Diss. ETH No. 14624
Investigation
of particles from combustion with
special
consideration of elemental carbon
A dissertation submitted to the
SWISS FEDERAL INSTITUTE OF TECHNOLOGY ZURICH
for the
of
degree
Doctor of Natural Sciences
presented by
Karl Richard
Przybilla
Dipl. Phys.
born
January 17,
citizen of
accepted
on
ETH
1973
Germany
the recommendation of
Prof. Dr. D. Pescia, examiner
Prof. Dr. H. Burtscher, co-examiner
Prof. Dr. H. C.
Siegmann,
2002
co-examiner
Dedicated to my parents.
Contents
Abstract
1
Zusammenfassung
3
List of Abbreviations
5
1
Introduction
7
2
Airborne Combustion Particles
11
of combustion
11
3
2.1
Properties
2.2
Health effects
15
2.3
Other effects
17
2.4
Particle mass,
2.5
Sources of airborne combustion
2.6
Tracing
and active surface
of combustion aerosols:
area
particles
significance
of elemental carbon
Methods
21
23
23
3 1 1
Dilution unit
24
3 1 2
Thermodesorber
25
3 1 3
Scanning mobility particle
3 1 4
Diffusion
3 1 5
Photoelectric aerosol
3 1 6
Gravimetry / coulometry
26
3 1 7
Bacharach soot number
26
Working
charging
area
25
sizer
25
sensor
25
sensor
27
measurements
Residential Oil Burners
29
details
4.1
Experimental
4.2
Results and discussion
29
42 1
Variation of burner
422
Variation of fuel
4 2 3
Non-optimal burning
4.3
18
19
Emission measurements
3.2
5
particle number,
Experimental
3.1
4
particles
30
30
type
33
conditions
-
influence of additives
Conclusions
34
40
Passenger Vehicles
43
5.1
Internal combustion
44
5.2
Experimental
5.3
Results and discussion
engine strategies
details
45
46
5.4
6
Stratified-charge
5 3 2
External
vs
vs
homogeneous-charge
46
47
to state-of-the-art passenger vehicles
48
Comparison
5 3 4
Validation of particle
diesel engines
5 3 41
Comparison
GDI
5 3 4 2
Total active
surface
5 3 4 3
Total particle number concentration
vs
50
measurements
sensor
51
53
area
vs
gravimetric total
mass
Conclusions
54
55
Area Measurements
57
6.1
Online detection of elemental carbon
57
6.2
Field measurement 1:
58
6.4
6.5
Bitburger brewery, Germany
6 2 1
Motivation and purpose of the measurements
6 2 2
Experimental
details
58
59
6 2 21
Test
run
1
ventilation at
62 2 2
Test
run
2
ventilation at full power
halfpower
59
59
6 2 3
Evaluation of the ventilation system
60
6 2 4
Results and discussion
61
Field measurement 2: Railroad tunnel construction site, Switzerland
6 3 1
Motivation and purpose of the measurements
6 3 2
Experimental
6 3 3
Results and discussion
Laboratory
details
measurement:
64
64
64
65
graphite particles
6 4 1
Motivation and purpose of the measurements
6 4 2
Experimental
6 4 3
Results and discussion
details
66
66
67
67
Conclusions
69
Conclusions and Outlook
Appendix
ii
mode
internal mixture formation
5 3 3
Working
6.3
7
5 3 1
71
75
A 1
Published material
75
A 2
Particle diameters
75
A 3
Measuring devices
77
A 4
Fuel and additive composition
78
A 5
Classification of oil burners
A 6
Calculation of the active surface
78
area
79
References
81
Acknowledgements
84
Curriculum Vitae
86
Abstract
Abstract
The
emissions of modern combustion systems
particulate
investigated.
consisting
Small-sized nucleation and accumulation mode
of elemental carbon
treated with
are
penetrate deeply into the lung and since they
diseases of the
respiratory
inside the human
therefore
emissions.
In
a
choose
Especially
consideration since
play
to
particles (diameter
an
important
they
correlate with the
atmosphere
meaningful measuring quantities
that
with
regard
particles
role with respect to
to very
small and
particle
on
able to
are
surface
area.
It is
particle
the basis of total
light particles
both
particles
for the assessment of
sampled
are
nm)
300
<
are
mass
this method may be
unfavorable.
a
first part, the
second part, the
vehicles
areas
and in the
Today, legislation requires
measurements.
quite
to
seem
with fossil fuels
and cardiovascular system. The effects of very small
organism
important
special
operated
are
particulate
emissions of
particulate
investigated.
In
emissions of three residential
a
third part,
with respect to elemental carbon
The
of
use
special
a
a
is
reduction of emitted
particles
used. In the
a
reduced
by
Gasoline
case
two
of
the air
yellow
for passenger
quality
accompanied by
case
of
at
working
can
misadjusted
the formation of
from the additive. On the other hand,
without side effects
conventional
examined. In
be achieved if
a
large
significant
highly purified
flame burner, the number of emitted
a
fuels
are
particles
is
orders of magnitude.
engines
purpose of fuel
monitoring
fuel additives achieves soot reduction in the
particles, stemming directly
are
presented.
residential oil burners. This effect is, however,
number of new
oil burners
direct-injection gasoline engine
method for
particles
light
with
savings
direct-injection
of fuel into the
and therewith reduction of
show, however, that direct-injection
can
C02
lead to
a
cylinder
are
being developed
emissions. The conducted
significant
for the
experiments
increase of soot
particle
emissions.
1
Abstract
By
high
means
of photoelectric
charging
of carbon
concentrations of diesel soot emissions
can
particles,
easily
the air
quality
at
be monitored. The
working
areas
applicability
with
of this
method for the detection of elemental carbon in ambient air is demonstrated with two field
measurements
2
and
a
laboratory experiment.
Zusammenfassung
Zusammenfassung
Gegenstand
dieser Arbeit ist die
Brennstoffen betriebener
Beurteilung
Vordergrund,
da sie eine hohe
Zeit im Verdacht stehen, im
im
menschlichen
zu
als
Organismus
<
mit
Die heute
anhand einer
Messung der
leichte Teilchen als
In
einem
spielen.
auch
Teil
in
Partikelemissionen
Da die
in
der
Fahrzeugbetrieb
Atemwege
mit
werden
die
an
Teilchen sowohl
Atmosphäre
allem
vor
gerade
von
untersucht.
Wirkung spezieller
Nebenwirkungen
Brennstoffe
mit
von
grosser
Partikelbelastungen
im Hinblick auf sehr kleine und
mit
In
dreier
einem
Leichtölbrenner
zweiten
Teil
Kraftstoff-Direkteinspritzung
zur
Benzinmotoren
Kraftstoffeinsparung
mit
um
aus
kann
zwei
zur
werden
die
für
den
Ueberwachung
Brennstoffzusätze wird
jedoch begleitet
dem Additiv
dagegen
gebildet
eine
am
von
Beispiel
der
einer starken Zunahme
werden. Durch die
deutliche
eines stark
Verwendung
Partikelreduktion
erreicht werden. Bei einem konventionellen Gelbbrenner lässt sich
Anzahl emittierter Partikel
der
Arbeitsplätzen vorgestellt.
sehr kleinen Partikeln, die direkt
reiner
und des Herz-
Wirkungen kleinster
Partikelemissionen
Benzinmotors
Russpartikeln
längerer
erweisen.
russenden Leichtölbrenners demonstriert. Sie ist
besonders
der
behandelt. In einem ditten Teil wird eine Methode
Die russvermindernde
an
aufweisen und schon seit
aussagekräftigen Messgrösse
Gesamtmasse kann sich
Eigenheimen
eines
elementarem Kohlenstoff stehen
Gesetzgeber vorgeschriebene Beurteilung
problematisch
ersten
Wärmegewinnung
Luftbelastung
vom
aus
Erkrankungen
Teilchenoberfläche korrelieren, ist die Wahl einer
Bedeutung.
nm)
300
Lungengängigkeit
Zusammenhang
eine zentrale Rolle
Kreislauf-Systems
Die besonders kleinen Nukleations- und
Verbrennungssysteme.
Akkumulationspartikel (Partikeldurchmesser
dabei im
der Partikelemissionen moderner, mit fossilen
ohne
so
die
Grössenordnungen vermindern.
Kraftstoff-Direkteinspritzung
und der damit verbundenen
Senkung
werden
der
zum
Zwecke
C02-Emissionen
der
entwickelt.
3
Zusammenfassung
Die
durchgeführten Experimente zeigen indessen,
einer markanten Zunahme der
Die
Belastung
der Luft
an
Arbeitsplätzen
photoelektrischen Aufladung
Eignung
dieser Methode
wird
Beispiel
4
am
zweier
Russpartikelemission
zum
von
Feldmessungen
von
Kraftsoff-Direkteinspritzung
zu
führen kann.
durch Dieselmotoremissionen kann mit Hilfe der
Russpartikeln
Nachweis
dass die
auf einfache Weise
überprüft
elementarem Kohlenstoff in der
und eines
Laborexperimentes
werden. Die
Umgebungsluft
demonstriert.
List of Abbreviations
List of Abbreviations
B
MAN burner
p. 31, table 3
BET
Brunauer-Emmett-Teller method
p. 19, section 2.4
BN
Bacharach soot number
p. 26, section 3.1.7
p. 25, section 3.1.3
CPC
condensation
d
diameter
DC
diffusion
DI
direct-injection
p. 9, section 1
DMA
differential
p. 25, section 3.1.3
EC
elemental carbon
ECO
highly purified
EL
extra
FGR
flue gas recirculation system
p. 30, section 4.2.1
particle
counter
p. 11, section 2
charging
p. 25, section 3.1.4
sensor
mobility analyzer
p. 8, section 1
extra
light
oil
p. 33, section 4.2.2
light
p. 21, section 2.5
GDI
gasoline direct-injection
p. 43, section 5
H
homogeneous-charge
p. 45, section 5.1
IDI
indirect
direct-injection
p. 44, section 5.1
OC
organic
carbon
p. 8, section 1
PAH
polycyclic
PAS
photoelectric
PMX
particulate
PS
metric
RPM
rounds per minute
p. 49, table 6
S
stratified-charge
p. 45, section 5.1
SA
surface
p. 8, section 1
aromatic
hydrocarbons
aerosol
matter
p. 25, section 3.1.5
sensor
with d
< x
p. 8, section 1
urn
p. 18, section 2.4
p. 49, table 6
horsepower
area
sizer
SMPS
scanning mobility particle
UV
ultraviolet
p. 26, section 3.1.5
Y
Giersch burner
p. 31, table 3
Y-R
Weishaupt burner
p. 31, table 3
p. 25, section 3.1.3
5
1
Introduction
Introduction
1
A
level of personal
high
features of
life, such
the
today's society.
physical
as
mobility
Elemental
health and
world
steadily increasing
and
a
high
capita
per
prerequisites
for
sound environment,
population,
energy
consumption
characteristic
are
untroubled and comfortable way of
an
are
often taken for
the side effects of human
granted.
activity
In view of
deserve close
attention.
A
of
large
fraction of small airborne
in urban
Inconsiderate
anthropogenic origin [1].
avoidable combustion
particles
particle
emissions and is
anthropogenic
The
the
combustion
accompanied by
of combustion
both persons and
millions of
means
of
widely
only
engines,
are
private buildings
cars,
serve
amounts
for the
and
monitoring
along
jointly responsible
dominated
adverse consequences in
the
limiting
-
emissions
6]
of
are
the purpose of
of fossil fuels
generation
are
of heat and
transportation
and diesel vehicles.
carried from
one
place
transportation. Heavy-duty
example,
but efficient
simple
for the fact that
by gasoline
goods
with the
buses, trucks, trains, ships, and airplanes.
used all around the world, for
Furthermore, large
causes
[2; 3] and environmental sciences [4
of fossil fuels,
and millions of tons of
motorcycles,
processes do not
availability
goods is, by far,
people
need of
systems
particles.
unlimited
seemingly
technology
for the
awareness
from combustion processes
of combustion
employment
different respects. Studies in the fields of medicine
have led to
stems
areas
to
Every day,
another
by
But combustion
diesel
for construction work in the
of
engines
are
building industry.
used in commercial industries, in
public
and in
electricity.
7
1
Introduction
In
the
theory,
produces only
stoichiometric combustion of pure
complete
carbon dioxide
(C02)
and water
(x |)-02
CxH^ +
+
Practical combustion systems, however,
xC02+|-H20
->
are
rarely perfect.
by-products
in gaseous
acid, ash). Insufficient mixture of fuel and
combustion zone,
example,
carbon
responsible
are
carbon monoxide
(EC)
and
(CO),
for
or
incomplete combustion, resulting
particles, consisting mostly
referred to
(OC), commonly
mechanical stress inside the combustion systems
For the
sake of
form
simplicity
combustion processes
legal
limits for
provide
are
particles
gravimetric analysis
development
100
neglected
particles
for
are
all based
on
particle
on
or
a
quite high.
long
Furthermore,
a
hydrocarbons (PAH).
Finally, high temperatures
and
can
be
parts).
means
particle
of
emissions of
measurements, and up to now,
mass
mass
This is
particle
[8; 9]. The
a
mass
is determined
by
that does not
collecting technique
number.
can
progress have led to the
be close to the detection limit of
the number of emitted ultrafine
Because very small
of, for
particles
have
only
particles (diameter
little mass,
they
have been
time. Recent health effect studies, however, have shown that ultrafine
potentially
indications that the
though
"soot".
additional material that
produce
of combustion systems whose emissions
even
inside the
of unburned elemental
practical alternatives, particle
samples [9].
size
well.
decades, environmental regulations and technological
is still
nm)
for lack of
usually judged by
are
gravimetric analysis [9],
<
or
of loaded filter
any information
Over the past
abrasion of metal
(e.g.,
as
as
gradients
in the emission
aromatic
polycyclic
Remnants of unburned fuel and lube oil may be emitted
particulate
non-
sulfates and sulfuric
(e.g.,
with temperature
along
multitude of hydrocarbon molecules is formed, e.g.,
emitted in
contaminated
are
and various
compounds,
form
particulate
oxygen,
and small
carbon
organic
sulfur
(e.g.,
Most fuels
The presence of fuel contaminations leads to the emission of
compounds [7]).
undesired combustion
(CxHy)
(H20):
with traces of elements other than C and H
combustible
fuels
hydrocarbon
more
surface
harmful
area
(SA)
than
of small
larger
ones.
Furthermore, there
particles (rather
than
mass) plays
a
are
strong
key
role in
toxicological respect [2].
Simple gravimetric analysis
particle
qualified
for
a
meaningful
emissions from combustion processes in the ultrafine size range
underlying
size distribution unfolds
considered here. There
8
of loaded filters is not
are
other
over a
wide range of diameters
measuring principles
that
serve
as
assessment
of
[9], especially
if the
it does in the
cases
this purpose better. In this
1
Introduction
work,
we
present
measurement are
In
chapter 2,
combustion
a
3
emissions from
particulate
is
given.
emissions
deals with
an
urn
used combustion systems,
widely
in diameter. Alternatives to the conventional
and evaluated.
applied
brief overview of the
particles
significant particle
Chapter
of
with sizes well below 1
emitting particles
mass
analysis
an
Relevant
are
properties
and
effects of small airborne
possible
measuring quantities
discussed and
are
of
sources
identified.
explanation
of the
experimental
methods for the conducted
measurements.
The
results of
experimental
burners and
on a
in
4 and 5.
chapters
where
6. The
comparison
Finally,
direct-injection (DI) gasoline
are
exposed to high
applicability
to
test
Selected parts of
three
of the
are
measuring principles
drawn and
chapters 4, 5,
of publication
an
generations
engine
are
outlook is
measurements at
used in the field
given
and discussed
working
particles,
are
are
verified
areas,
given
by
in
means
well controlled conditions.
in
chapter
and 6 have been considered for
can
of residential oil
presented
concentrations of combustion
laboratory experiments, performed under
conclusions
respective places
measurements on
Furthermore, examples of air quality
working people
chapter
of
modern
particle
be found in section A.l of the
7.
publication.
Details
on
the
appendix.
9
2
Airborne Combustion Particles
Airborne Combustion Particles
2
Ambient air consists of
diameter
d,
distribution
from
ranges
as a
a
•
accumulation mode
(d:
mode
|im)
example
of
an
(d <
(d >
1
distribution in
of
figure
accumulation and
30
50
-
by
300
Their size,
specified by
(b),
coarse
of ambient air
can
usually
be
shape:
nm)
size distribution is shown in
nucleation mode
This
where the volume
particle
their
of micrometers. The number
tens
some
Aerosols
particles (aerosols).
sources.
arbitrary sample
an
particle
larger-sized particles.
1
solid
nm)
average urban air
number is dominated
composed mostly
or
linear combination of three different modes of lognormal
nucleation mode
coarse
anthropogenic
size of
particle
•
•
particle
suspended liquid
few nanometers to
a
function of
approximated by
An
of
from many different natural and
originate
well
variety
a
The
particles.
can
be
seen
particle
from the
(proportional
to
mass)
figure
mass,
1
(a).
The
however, is
corresponding
volume
is concentrated in the
mode.
Properties of combustion particles
2.1
Combustion processes contribute
substantially
air, especially in the vicinity of urban
those
employing
See section A 2
gaseous
m
the
or
areas
[1].
to
the amount of
for
an
explanatory
found in ambient
Most modern combustion systems,
liquid fuels, produce mainly
appendix
particles
remark
on
particularly
nucleation and accumulation mode
particle
diameters
11
2
Airborne Combustion Particles
(a)
Number
(b)
Volume
Total Concentration
Total Concentration
Accumulation
Particle Mode
Nucleation
Particle Mode
Coarse Particle
Mode
-
(not visible)
'
0 01
0 1
1
Particle diameter d
Example of
Figure
1.
usually
resembles
a
an
0 001
investigation
coarse
to
linear combination of three separate
tear
liquid hydrocarbon
composition
mixture of many different
duty
diesel
engine
is
12
nucleation mode
accumulation and
coarse
neglected
from
distributions,
possibly
the
compounds.
use
mode
In table
displayed. Depending
on
1,
are
and diesel
impurities,
significant
particles
typical particle composition
listed in table 1
can
our
engines.
wear
and
factors that
therefore consist of
the combustion system and the
respective components
The number
We further restrict
gasoline engines,
Combustion
a
(a)
particles.
now on.
of fuel additives
particles.
[1]. The shape
particles, (b) The corresponding
of unburned fuel and lube oil, fuel
of combustion
the fractional amount of the
lognormal
fuels for oil burners,
remnants
of mechanical parts, and
influence the
by
by
mode shall therefore be
Incomplete combustion,
1
T^ml
average urban aerosol size distribution, taken from
volume concentration is dominated
The
0 1
Particle diameter d
concentration of urban aerosol is dominated
particles.
0 01
T^ml
vary
for
a
a
heavy-
operating mode,
widely.
2
Airborne Combustion Particles
Component
EC
41 %
Incomplete combustion
Hydrocarbons
32%
Unburned fuel and lube oil;
Sulfur compounds
14%
Water
13%
Ash and other
Table 1.
heavy-duty
transient
combustion
systems
cycle.
or
solid
Metal
conversion) [1].
particles
and
compounds (sulfate
constituents
delicate
compounds
emitted
they
sulfuric
product; condensation
in fuel and lube
by
a
heavy-duty
diesel
[10]. The composition
are
either emitted
of EC,
zone) by homogeneous
In the latter case,
combustion
oil, (and additives);
can
engine, operated
vary
widely for
in
a
other
modes.
nanoparticles consisting mostly
outside the combustion
ordinary
mechanical abrasion
Data taken from
operating
incomplete combustion
Sulfur traces in fuel and lube oil
Water:
Typical composition of particles
Nucleation mode combustion
as
Origin
Fraction
consist
acid)
and
they
or
are
from the combustion
zone
formed in the exhaust stream
(i.e.,
directly
nucleation of gaseous material
mainly
of volatile
[10; 11]. Sampling from the hot exhaust
material and sulfur
droplets, usually
as
emerge
organic
(gas-to-particle
without
gas of combustion systems is
task, because the extraction and dilution procedure
can
a
solid
very
trigger homogeneous
nucleation, thereby changing the number of nucleation mode particles significantly [9; 10].
Figure
2 shows
an
example
of how the dilution process
Except for the dilution ratio, both spectra
the dilution ratio between
possible
that
large
raw
2
exhaust and diluted
obviously
respective sample considerably.
humidity
figure
are
can
alter
particle
is not
particles
high enough (curve A),
are
increases the number, SA, and
formed
mass
it is
by homogeneous
concentrations of the
At constant dilution ratio and exhaust temperature, similar
also be caused due to the dilution air temperature,
of the dilution air
size distributions.
recorded under identical conditions. If
sample
numbers of small nucleation
nucleation. This effect
nucleation effects
in
can
[12].
In real world situations
(i.e.,
or
due to the relative
dilution of
raw
exhaust in
13
Airborne Combustion Particles
2
10'
Nucleation Mode
'Particles
A
A
D
B
-
-
Dilution Ratio 1
:
20
Dilution Ratio 1
:
50
10°
10
10'
o
Ü
10
10
10
100
Electrical
Figure
partial
of
2.
Particle size distributions, measured
amounts of nucleation mode
The
dilution
factor must be
formation of nucleation particles
ambient
air),
nucleation mode
natural dilution conditions
are
generally performed
can
particle
vary
sufficiently high
(B).
Data taken from
effects
with the intention of
dilution in ambient air. Generation of
reflecting
the combustion
cause
engine
with
a
generation
the
in
order to
avoiding
particle
inhibit the
[12].
can
the emission measurements
greatly,
arbitrary
very well
presented
occur.
As
in this work
additional formation of nucleation
information inside the
post-combustion
raw
nucleation
exhaust, before
particles
can
be
experimentally by:
•
•
•
choosing sufficiently high
dilution ratios
pre-heating
the
dilution air
controlling
the relative
It is worth
mentioning
particle-free
nucleation
particle
humidity
of the dilution air, where
that both fuels with
(traps, catalysts) promoting
the
S02
—>
high
appropriate
sulfur content and after-treatment devices
SO^ formation, greatly
enhance the
tendency
of
formation.
In the context of combustion
14
TDI diesel
described above
as
thus
soot
on a
particles by gas-to-particle conversion
particles,
avoided
[nm]
stream dilution tunnel. Insufficient dilution ratios
high
(A).
Mobility
1000
Diameter d
the accumulation mode is often referred to
particles,
mode. Particles from this mode
are
usually single
or
agglomerated
solid EC
as
the
particles.
Airborne Combustion Particles
2
While the
primary particles
themselves
A
are
filled and the
typical
surrounded
can
structures
particle
consists of
ratio between solid and volatile
and fuel
removed
prior
(section 3.1.2).
combustion
This
can
The
large
by heating
be desired if
may lead to
loads of diesel
those
vulnerable
It is
particles
can
or
is
mainly
agglomerates,
hollow
agglomerated particles),
coverage with
the
on
adsorbates, i.e., the
combustion system,
particle
thereby evaporating
Experiments
particles
with
particles
constituents
the volatile
can
be
compounds
interested in the solid fraction of
from
be inhaled and
inflammatory responses
the influence of certain
and
cause
anthropogenic
deposited
considerable
in the
is
sources
a
threat to
respiratory tract,
damage
the
to
where
respiratory
conducted with animals have proven that exposure to
causes cancer
[2]. Adverse health effects
co-pollutants (e.g., ozone) [2].
and
compromised respiratory
Sensitive
are
greatly
systems,
high
enhanced under
people, especially
cardiovascular
and
the
elderly
particularly
are
[2].
important
to
distinguish
completely different,
•
•
once
they
between two components of inhaled
are
deposited
that behave
organism [1; 9]:
insolvable solid components
deposited deeply
inside the
thin alveolar membrane
are
deposited
lung, they
can
6, page
in the human
enter
[1]. Consecutively, they
Age and surrounding of emitted particles have
section 2
inside the human
nanoparticles
solvable components
The solvable components that
*
(single
Volatile
.
clusters of grapes
or
shape [14].
core
content)
and
one
number of airborne combustion
cardiovascular system.
are
in
agglomerates
particles.
human health, since small
and
spherical
of
case
the
Health effects
2.2
they
in the
[14]. The surface
sulfur
shape,
branched chains
particles;
solid EC
a
in
spherical
fraction, depends strongly
purity (e.g.,
to measurement
rather
resembling
more
adsorbed volatile material
operating mode,
are
condense onto
particles become
combustion
by
agglomerates
complex
can assume
[1; 13]. Volatile material
spaces
of
a
organism
are
dissolved. If
they
the bloodstream after
passing through
the
diluted and
all
the
are
significant
influence
on
the
dispersed
over
particle properties
See
21
15
2
Airborne Combustion Particles
Given this
organism.
solvable substances is
solvable
of distribution, it is reasonable to
pathway
proportional
from
components stemming
dangerous substances,
Inhaled and
differently
such
foreign
tract
depends
is
equipped
life.
likely
the
on
that
some
Very small particles
where
they
are
PAH
are
processes
many
exist
small EC
as
well.
behave
particles)
reasons:
with several clearance mechanisms for insolvable
particle
size.
The
inside the
particles
from
are
not
a
couple
respiratory
deposition,
combination of these
particles varying
particles
which
factors creates
of hours to several years
removed at all and remain in the
body
for
believed to be able to enter the blood circulation from
are
transported
Although
(e.g., benzo-(a)-pyrene [15]),
(e.g.,
of
toxicity
presumably non-toxic,
the clearance mechanism and the location of
on
residence times of removable
It is
combustion
The residence time of inhaled
matter.
depends mainly
[1].
that has been taken up.
than solvables for two main
organism
solid
mass
insolvable solid components
organism
1. The human
the
carcinogenic
as
deposited
in the
to
that the
assume
other organs
to
[2; 16]. They
may be involved in
clogging
of very fine arteries.
2. There
are
strong indications that the SA of inhaled solid particles is the key quantity
related to health
laboratory
effects.
animals show that there is
the correlation with the
particles possibly
In
figure 3,
human
the
respiratory
for
probability
probability
tract
point
deposition
mode
In
can
in these two
catalyst
for
particle
of small nucleation
especially
be
seen
regions
good
correlation with the
mass
specific
in the alveolar
from
lies
figure
exactly
whereas
[2]. The
SA of
of inhaled airborne
is
high
region
nm
more
3 that the maximum
in the
and 10 |im. While the
in the head
is far
particles
airways, deposition
serious from
probability
for
a
health
respiratory
in the size range of nucleation and accumulation
particles.
conclusion, the threat from combustion particles imposed
combined facts that
particle
on
human health relies
emissions from modern combustion systems,
significant
effects, and high probability of particle deposition deeply inside the lung all
range of nucleation and accumulation mode
16
induced in
particle SA,
is less evident
diameters between 1
particles
tumors
reactions with cells.
respiratory deposition
is shown for
deposition
of view. It
for
a
respective particle
acts as a
in the tracheobronchial and
effect
Dose-response analysis from lung
particles.
occur
on
the
health
in the size
2
Airborne Combustion Particles
2.3
3.
human
respiratory
tract. Data taken from
inhaled
particles inside the
[1].
Other effects
Combustion
climate
Probability for respiratory deposition of
Figure
particles play
effects.
condensation
combustion
Clouds
a
are
composed
of water vapor
particles
into the
role in connection with environmental
of small
condensation
on
water
nuclei.
atmosphere provides
which
droplets
The
pollution
emission
are
of
and
possible
formed
by
anthropogenic
additional condensation nuclei which
promote the formation of clouds with adverse properties concerning scattering and absorption
of solar radiation. Possible consequences
suppression
particles
SA
changes
in the
atmospheric temperature structure,
of rainfall and less efficient removal of pollutants
Airborne combustion
particle
are
can
and
serve
S02
particles participate
the purpose of
in the
atmosphere,
sulfuric acid. Sulfuric acid is not
known for its
deteriorating
effect
catalyzing
for
only
on
in the
example,
atmosphere's
chemical processes,
chemical reactions
fosters the
[5]. The
catalytic
the
as
concurrence
conversion of
S02
of
into
harmful for humans upon inhalation, it is also well
buildings
reinforced concrete, corrosion of steel,
[4].
and construction materials
crumbling
of
(e.g.,
corrosion of
facades) [17].
17
Airborne Combustion Particles
2
2.4
particle number, and active surface
Particle mass,
area
threshold limit values for
Today,
in terms of
emissions.
method for determination of the
mass
undertaken. This
In terms of size
is
particle
particle size,
to
allows
procedure
a
by
the
of
particles
composed only
(light) particles (d « x)
proportional
collected
according
of
particles
d
to
standard:
respective PMX
have been
particle
accumulation mode
number. In many
the
few
only
deposited
.
particles.
on
the filter
atmosphere
mass.
The
These
is also
particles
small in
are
mass
PM2
**
5
=
=
18
the
particle's
of both number and volume
a
simple
insensitive to number
mass
only particles
only particles
The reduction of
l e
,
PMX,
particles.
to
the collected
or
x.
It
many small
or
with d< 10
with d
large
of those
<
mass
(proportional
a
particles
with d
(during
mass)
> x
reasonable
hand, the
particle
by
the
distribution
polydisperse particle
to
particle
particle
(figure
distribution is
the small-sized side of the
u.m, prior to filter
deposition
collected
u.m are
collected
and thus
heavy particles (d >
particles
visible to the naked human eye
1
u.m)
has
SA
Interaction of particles
rather than
to
in
high
On the other
mass.
the
nucleation and
has shown that the
properties,
of
mass
[9].
spectrum
thereby reducing
but often
particle
SA, especially with regard
u.m are
2 5
mass
particle
SA
emission
produce mainly
particles
measurement
standard demands precipitation of all
visible soot,
be
can
spherical particles,
particle
detection limit
effects than does the
governed by
1, page 12) underline that
PM10
that for
the
changed
cases, the amount of collectable
dose-response
comparison
PMX
(note
Modern combustion systems
is in the range of the
correlates better with
in the
definition of
by
large (heavy) particles (d~x)
discussion about health effects of small combustion
The
from smaller sized
size towards smaller diameters and
particle
mass
practical
measuring periods)
*
standards
).
significantly by shifting
completely
standardized
a
In order to relate
[9].
PMX
to
particulate
with diameters smaller than the cut-off diameter
Improvement of combustion systems has
total emitted
loaded filters
on
coarse
gaseous and
gravimetric analysis,
size selection
separation
remains unknown, however, whether
is
mass
on
defined
generally
are
classification, the information obtained from gravimetric analysis is limited
the size interval defined
mass
[8]. This applies for both
of particulate emissions is based
Judgement
the collected
(|ig/m3)
concentrations
mass
substances
specific airborne, (toxic)
essentially
resulted
m a
reduction of
2
Airborne Combustion Particles
spectrum. In view of these facts, it
on
particle
number and the
particle
should be observed in addition to
It has been
health effects caused
geometric
SA of
SA that is
directly
and cavities
out in
pointed
are
respective particle
particle
be determined
can
This
measuring
on
by
a
reducing
the
required mass
based
on
time resolution
electrical
atoms to
charging
attachment
cross
information
as
from the gas
charging
2.5
means
in terms of
key
role with
regard
the
distinguish
to
(total)
geometric
by
of the Brunauer-Emmett-Teller
sources
pores
nitrogen
on
This
the surface of
[19; 20]. This
amount
increases the
10
a
mg).
nitrogen,
sensitivity,
of matter is still very
high
are
therefore not very
practical,
and measurements
impossible.
are
aerosols.
Labeling
respective
on
can
the attachment and measurement of labeled
be achieved either
molecules
or
atoms.
section of the aerosol. The attachment
phase [20].
>
Kr instead of
technique
(BET)
examined in this work. SA measurements of aerosol
the BET method
of the
decay.
adsorption
In this
kinetics and
by
This
cross
radioactive
marking
principle depends
section includes
particle growth by
work, the active SA is measured by
or
on
by
the
important
attachment of material
means
of
a
diffusion
(section 3.1.4).
Sources of airborne combustion
Legislation
a
we
of radioactive
adsorption
of samples to 1 mg
it determines
sensor
following,
the amount of adsorbed
Determination of the active SA relies
or
by
of the radioactive
measurement
for the combustion aerosol
molecules
In the
plays
analysis requires, however, relatively large samples (mass
followed
high
mass.
particles.
A variation of this method involves the
with
that
important quantities
are
disregarded [20].
given sample [19].
are
particles suggests
accessible from the outside, i.e., "hidden" inner surfaces created
method, which is based
that
requirements
from the active SA: the active SA is that fraction of the
particles
The geometric SA
samples
SA
section 2.2 that the SA of particles
inhalation of
by
and necessary to extend the
appropriate
The mode of action of small airborne combustion
measurements.
that both the
seems
particles
in Switzerland defines threshold limit values for airborne combustion
mass
concentrations per unit volume of exhaust gas
officially approved sampling
method is
gravimetry,
limited to the
particles
(|im/m ) [8]. Today,
PM10 fraction,
even
the
though
19
2
Airborne Combustion Particles
epidemiological
related effects
1995
the
this
available, it is
1.
by
of combustion
occurrence
at
PM2 5-based
[21]. The primary PM10 emissions
commissioned
study
Since,
studies indicate that
in
point
airborne
that
are
important
points
means
larger
that
only
-
than 2.5 |im.
meteorological
of the
15
30 % of the
or
due to
presented
sample,
ultrafine
it is
particles
and is
magnitude
emit
knowing
of
Switzerland
85 % of the
PM10
This
mass.
of ambient air
normally
are
are
of the data:
interpretation
large primary particles
the collected
mass
is
PM10
specific
are
due to unusual
in the
vicinity
mean
only
emits
that the
ultrafine
only
mass.
particles
Figure
source
particles,
in
can
question
like the
is
the contribution of
(page 12)
1
of few
specific PM10
can
not
serve
as
an
large-sized (heavy)
be, however, higher by orders of
small amount of
negligible.
sources
attention, precisely because they do
on
a
in connection with health effects
comparatively
a
in the size range of well
predictions
usually composed primarily
especially important
source
particles
the size distribution of
make reliable
to
The number of very small
particles.
does not
impossible
to
indicator that the
a
-
across
PM10 samples
in this work deal with
below 1 |im in diameter. Without
If
sources
related to
sampling point.
2. All measurements
mass
found in
particles
for
deviations from this ratio
Significant
conditions
particles
fraction accounts for 70
5
are
a
discussed in this section.
are
on
[21], the PM2
to
in ambient air
time, only PM10 data
necessary to stress two
According
Switzerland have been assessed in
across
[21]. Conclusions from this study that
BUWAL
particles
correlate better with health-
measurements
(section 2.2).
PM10
On the contrary,
presented
in this
stand out from
PM10
matter, this
sources
that
work, deserve close
data and
are
easily
overlooked.
In table
2, the percentage contributions of specific
in Switzerland in
1995,
are
listed
according
further subdivided. Note that the
origin, i.e.,
not
only
combustion
small fraction thereof. For
PM10
particles.
example,
to groups
mass
The
PM10
40.6 % of the
*
20
Bundesamt fur
engines,
to
the total
PM10 mass,
of sources. The individual
measured
sources can
be
referred to in table 2 contains matter of any
exhaust emissions. This includes all gaseous and
from road traffic stemmed from diesel
sources
mass
from combustion processes is
PM10
particulate
mass
Bern
a
from road traffic stem from
emissions. If all exhaust emissions
the EC content would
Umwelt, Wald und Landschaft, CH-3003
only
again be
another fraction
2
Airborne Combustion Particles
thereof
(approximately
into
apportioned
not
determination
involving
table 2
and
can
chapter 4),
can
for
not
larger
see
table 1, page
combustion
contributions
be
given.
from
13). Unfortunately,
case
estimates based
of residential extra
the contribution to
PM10
mass
sources
on
light (EL)
is
PM10
data from
instance,
combustion
specific
the
for
products like,
given here, only rough
For the
example,
2.8 % listed in table
%,
typical
of the
be
41
is
the total
therefore
PM10
oil burners
again only
a
precise
A
EC.
[21] is
mass
very
from
(examined
in
small amount of the
2, since household furnaces using other types of fuel (coal, wood) emit
and thus heavier combustion
particles.
Group
% of total
Source
Road traffic
Traffic
(passenger
and
freight traffic),
36.4
off-road traffic
Energy supply
PM10
Total
0.4
Furnaces
2.8
Other
1.7
Households
Industry
and trade
Agriculture
and
forestry
Total
35.0
Total
23.7
Total
100
Table 2. Sources of
2.6
Tracing of
PM10
matter in Switzerland. Data taken from
combustion aerosols:
[21].
significance
of
elemental carbon
Combustion
particles undergo
Interactions between
SA
particles
several
changes
and molecules from the gas
properties (e.g., condensation, adsorption,
collide with each other
can
once
or
they
are
emitted into ambient air.
phase change
evaporation
of gas
the
particle's
molecules).
chemical
Particles that
coagulate ("stick together"). Coagulation increases particle
size and
21
2
Airborne Combustion Particles
reduces
particle
number.
composition governing
pitfalls concerning
In the
EC is
case
always
on
the
this
properties
measurement
there is
no
conservation
of aerosols. This fact creates
and data
interpretation
related to combustion processes, and the
products,
conserved with
combustion aerosols
are
of aerosols in
following chapters.
good
a
or
comparison
of
a
mass
mass
or
number of
chemical
potential
general.
reliable tracer. The
occurrence
of
of emitted EC is, in contrast to
accuracy. Air
therefore often undertaken with
For this reason, the detection of EC
22
sense,
of combustion aerosols, EC has proven to be
other combustion
focus
In
quality
special
measurements
with
consideration of EC.
of other data with EC will be stressed in the
3
Experimental Methods
3
Experimental
In the
following,
we
distinguish
"tailpipe" measurements,
devices
measuring
3.1
can
Methods
and
between two types of measurements,
working
area
measurements.
be found in section A.3 of the
namely
Additional information
emission
on
or
the used
appendix.
Emission measurements
In emission
or
"tailpipe" measurements, samples
of combustion systems.
Depending
on
the
are
respective
taken
directly
from the hot exhaust gas
combustion system, the exhaust gas
reach temperatures of several hundred °C. It is necessary to dilute the
raw
can
exhaust in order to
avoid condensation effects while the exhaust air cools down, and in order to not exceed the
range of the
measuring
provide
measurements
employed measuring
devices. It is
important
information about "fresh" aerosols. Once
been diluted in ambient air,
they
subject
are
to
various
to
particles
ageing
realize that emission
are
emitted and have
processes that
can
alter their
properties considerably (section 2.6).
4 shows
Figure
a
following chapters.
means
of
a
rotating
schematic arrangement for the emission measurements
The
sampling
in
a
thermodesorber
consisting
of
a
(section 3.1.4),
(section 3.1.1). Depending
to remove
(section 3.1.2).
large
a
photoelectric
amounts
on
the
aerosol
respective
of volatile material
After that, the aerosol is fed into the
scanning mobility particle
and
in the
volume is extracted from the center of the exhaust line
disk dilution unit
system, it may be necessary
presented
sizer
(section 3.1.3),
sensor
(section 3.1.5).
a
prior
by
combustion
to measurement
measuring equipment,
diffusion
charging
sensor
23
3
Experimental Methods
From
a
deposited
separate measuring point, samples of
on
filters for
3.1.7)
and coulometric
gravimetric (mass)
In the
content) analysis (section 3.1.6).
case
is measured instead of gravimetry /
exhaust
raw
extracted, diluted and
are
(inorganic
and
organic
of oil burners, the Bacharach soot number
carbon
(section
coulometry.
11
to
CD
CO
(A)
Photoelectric Aerosol Sensor
(4)
Diffusion
Undiluted
(1)
E
(5)
'Stream
/
(B)
„
Charging
Sensor
Diluted
Stream
Cß
3
CO
'
X
LU
Heating
\
Coohng
Thermodesorber
(2)
\
c
o
CO
=
c
o
Fuel
Figure
Gravimetry
E
f
Coulometry
Pump
Bacharach Soot Number
>,
o co
4.
extracted
Experimental setup for emission
(A) by
means
aerosol stream passes
is then fed in
of
a
rotating
through
a
measurements. The flue gas is
disk dilution
thermodesorber
system (1). The diluted
(2) (only
if
necessary)
parallel into the measuring equipment, consisting of
mobility particle
aerosol
/
or
a
sensor
sizer
(3),
a
diffusion
Flue gas for
(5).
charging
gravimetric
sensor
(4),
and
and coulometric
a
a
and
scanning
photoelectric
analysis,
determination of the Bacharach soot number, is extracted from
a
or
for
separate
measuring point (B).
3.1.1
Dilution unit
The extracted hot exhaust gas is diluted
Dilution unit and
adjustable
24
particle-free
between 1:10 and
dilution air
1:104.
by
can
means
of
a
rotating
disk dilution unit
be heated. The dilution ratio is
[22].
continuously
3
Experimental Methods
3.1.2
Thermodesorber
The first part of
a
thermodesorber
up to 400 °C. While solid
evaporated
from the
particles
particle
[11] consists of a tube that
pass
through
the heated area, adsorbed volatile material is
surface. In the second part, the aerosol stream passes
water-cooled activated charcoal trap. Here, the volatile
solid
particle
A
fraction remains in the stream and
Scanning mobility particle
3.1.3
scanning mobility particle
sample [25].
To this
sized in
differential
a
appendix A.2)
are
A diffusion
a
sensor
charged particles,
proportional
to
the total active SA
obtain the total active SA of
down to
one
3.1.5
(d<
1
a
properties
the
defined size
particle
measures
created
particle
measuring equipment.
size distribution of
their electrical
to
aerosol
an
equilibrium charge. They
are
then
mobility.
(electrical mobility equivalent diameter,
counter
(CPC).
the total active SA
by
electrical
properties.
corona
insulated filter, is measured
[23].
given
It is therefore
aerosol
Photoelectric aerosol
|im)
stripped
possible
sample directly.
(section 2.4)
Particles
discharge.
electrically.
to
are
of small
charged by
The current of
The DC
signal
is
calibrate the DC in order to
The DC has
a
time resolution of
second.
photoelectric
A
an
The
a
sizer
of their chemical surface
polarity,
collected in
captured.
through
sensor
(DC)
particles (d<\ |im), independent
one
a
are
be fed into the
first neutralized to
are
condensation
charging
charging
attachment of ions of
can now
(SMPS) yields
of
particles
counted in
Diffusion
compounds
mobility analyzer (DMA) according
the selected
3.1.4
sizer
end, the particles
Subsequently,
be heated to temperatures
can
from
aerosol
sensor
sensor
(PAS)
incomplete combustion,
of aerosols,
composed
is well suited for the detection of small
due to its
of EC and
high sensitivity
particle-bound
PAH
to
particles
the chemical surface
[23; 24].
A PAS
measures
the
25
3
Experimental Methods
electrical current of
charged by
emission of
removed in
a
photoelectrons
upon irradiation with UV
depends
surface and is sensitive to chemical
resolution of down to
material is
weighed
conditioned
thereby deposited
before and after
of coulometric
and total OC
analysis,
mass
on
particle
are
positively charged
the work function at the illuminated
of the
changes
photoelectrons
particle
surface. The PAS has
a
time
filters.
on
a
defined volume of diluted exhaust gas is sucked
Particulate
the filter. In the
loading.
This
the filters
are
the
yields
condensates
(and possibly
of
case
gravimetric analysis,
the total accumulated
analyzed chemically
legally approved
concentrations of airborne
3.1.7
analysis,
particle
of
volatile)
the filters
mass.
In the
are
case
for determination of the total EC
[26].
is
Gravimetry
particulate
standard
testing procedure
for
judging
mass
matter.
Bacharach soot number
The Bacharach soot number
of combustion, based
deposited
on a
combustion
filter
quality
on
the
(BN)
is
a
qualitative
optical absorption
[27]. The
of visible
BN is part of the
of oil burners,
as
defined
by
measure
a
discolored spot. The color of the spot is
0
(white)
to 9
light
(black).
Swiss
shone
on
compared
This number is assessed
the loaded filter. The
evaluating
the
light by particles
completeness
that have been
the
legislation [8].
with
through
a
a
white filter,
calibrated gray scale
electronically by measuring
discoloring
presence of black soot which is assumed to be
for
required testing procedure forjudging
A well defined amount of undiluted flue gas is sucked
26
the
second.
one
and coulometric
gravimetric
through specially
visible
light;
are
Gravimetry/coulometry
3.1.6
For
insulated filter. Particles
an
weak electric field in order to prevent recombination with
Emission of photoelectrons
particles.
collected in
positively charged particles,
of the
sample
composed mainly
leaving
behind
reaching
from
the reflectance of
filter is attributed to the
of EC.
3
Experimental Methods
3.2
Working
Working
Samples
already
are
engines
are
in
concentration at
•
•
•
•
The
cooled down to ambient air temperature and is diluted to
the purpose of
concentrations
•
differ from emission measurements to that effect that the
taken from ambient air rather than
measurements serve
particle
measurements
measurements
area
aerosol has
area
can
be
and
use)
working
expected (e.g.,
where
areas
evaluating
depends
spacial particularity
the air
of the
on
health
many different
working
area
type and capacity of ventilation (natural
spacial
number and
area
spacial
of air
particle
ambient air and
2.6
(page 21),
yielding
to
is
therefore
factors,
(indoors
vs.
vs.
where elevated
heavy-duty
risk.
at
The
of which
some
outdoors,
room
diesel
aerosol
are:
geometry)
artificial)
distribution of particle emission
measurements
compared
EC is
working people
areas
filters
presented
in this work
of the PAS at different locations. Dilution of the
measured data is
working
at
These
source.
distribution of fresh air and exhaust air ventilation shafts
separation efficiency
working
quality
emitting
construction sites where
at
occupational
from the
directly
extent.
some
a
the
to
performed solely by operation
volume
analysis
concentration of EC. For the
standardized
combustion
sampling
conventional coulometric
mass
are
sources
quantity
for
occupational
was
not necessary.
of filter
reasons
health to
samples,
The
taken in
mentioned in section
assess
the exposure of
particles.
27
4
Residential Oil Burners
Residential Oil Burners
4
In
They
developed countries,
the purpose of
serve
residential oil burners
can
providing
for
warm
water
temperatures, especially during the cold winter
year round for
In this
general
household activities
three
chapter,
generations
ultrafine
particle
ultrafine
particles according
Photoelectric
of
particles.
charging
operated
performed during
the
investigated
with respect to
characterizing
(chemical)
qualitative interpretation
state
work).
the emitted
diameter and number concentration.
sensitive to the
steady
home.
is, of course, also used all
operating
surface
properties
of additive effectiveness.
condition. All burners
with two different types of EL oil and with different concentrations of
fuel additive
4.1
are
mobility
are
are
private
heated at comfortable
kitchen
the purpose of
serve
charging
The BN is measured for the
Measurements
Warm water
season.
(e.g., personal hygiene,
their electrical
and diffusion
keeping buildings
of residential oil burners
emissions. Size spectra
to
be found in almost every
a
are
prominent
(ferrocene).
Experimental details
The measurements considered here
gas is extracted 7
ratio is 1:300, the
to remove
sheath air
m
vs.
emission measurements
behind the burner where it has
presented
volatile
are
data
compounds.
1.5 1/min. aerosol
are
a
(section 3.1).
The exhaust
temperature of 65-75 °C. The dilution
corrected for dilution. A thermodesorber is used at 330 °C
The SMPS system is
flow), leading
to a
operated
particle
in
high-flow
size range of 6
-
mode
220
(15
1/min.
nm.
29
4
Residential Oil Burners
The flue gas of the burners is lead away
by
of
means
ventilation system which
a
provides
a
but constant pressure difference between the stack and ambient air. This makes the
slight
system independent of influences from changing weather conditions.
The burners
each
of fuel, the oil filter,
change
burner is
with different fuels and ferrocene additive concentrations. For
operated
are
for 30 minutes before
operated
and oil canisters
tubing,
heat
of the
exchanger temperature
order to
provide
the best
One burner is
coulometry,
4.2
on
a
in
BN not
In
higher
only
the
BN is
brought
defined temperatures in
to
data
are
measured in the
start).
produces high particle
measured instead of
emissions
gravimetry
required testing procedure forjudging
the combustion
Switzerland, residential oil burners
must
than 0.5
the fuel and additive
and the
after both the boiler and the
presented
mode that
thoroughly
conducted.
20 minutes after burner
a
this case,
In
All
cleaned
/
quality
fulfill the
legal
[8].
composition
can
be found in section A.4 of the
appendix.
Results and discussion
Variation of burner
4.2.1
Three
generations
conventional
is also
ratio).
oil burners.
of
requirements
Details
(approximately
since it is part of the
of residential
circuit have been
deliberately operated
air-fuel
(misadjusted
cooling
conducted
are
possible reproducibility.
condition
stationary operating
measurements are
new
The burner is started and measurements
are
a
yellow
yellow
burner),
of burners have been
flame oil burner
flame burner,
for reduction of
NOx
which is
type
compared (table 3).
(yellow
to
burner).
additionally equipped with
emissions. The MAN
supposed
flame
produce only
emissions. See section A.5 in the
(B)
a
burner is
The Giersch
The model from
for
more
burner is
a
blue flame oil burner
information
on
a
Weishaupt (Y-R)
flue gas recirculation system
very little soot and which is
appendix
(Y)
optimized
(blue
(FGR)
flame
for low
NOx
the classification of oil
burners and FGRs.
The ultrafine
particle
emissions of all three burners
particles
with diameters between 6
therefore
incomplete, especially
30
at
-
220
nm
are
are
plotted
in
figure
5. Note that
measured and that the size spectra
only
are
the small-sized end of the spectrum. The burners Y-R and B
4
Residential Oil Burners
Label
Specifications
Model
Y
yellow flame
Giersch R1-V
Y-R
yellow flame
Weishaupt
with FGR
WL10-B-H-1LN
blue flame
MAN Raketenbrenner
B
low
N0X
RE 1 LN
Table 3. Examined residential oil burners.
Figure
5.
Comparison of
the
particle spectra of three different burners. See
table 3 for the definition of the burner nomenclature Y Y-R, and B. Lines
without markers represent the cumulative
sum
of particles
on a
linear scale
(right axis).
show
(B).
a
significant
The total
stemming
particle
case
increase of the
particle
from
number is
particles
particle
highest
smaller than 30
number at diameters below 30
for the blue flame burner B, the
nm
in diameter. For diameters
number of the blue flame burner B is up to
of the
yellow
nm
one
(Y-R),
major
larger
and 50
nm
contributions
than 30 nm, the
order of magnitude smaller than for the
flame burners.
31
4
Residential Oil Burners
In terms of mass,
figure 6,
where the
constant
density),
particle
the
particle
is
volume concentration
plotted
as a
is calculated from the
particles
particle
however, the picture looks somewhat different. This
are
spheres.
mass, the
mobility
function of the electrical
respective
electrical
The conventional
significant
diameters of 70
nm
increase of
and
flame burner with FGR, Y-R, is
(proportional
mass
larger.
clearly
yellow
particle
high
mass
amount
of very small
6.
Comparison of
concentration) of
stemming
The emitted
The filter
BN of 0.5
blackening
or
by
One has to
yellow
particles (figure 5),
investigated
in
a
from
assuming
assumption
highest
mass
of the advanced
a
that
amount
larger-sized particles
of
with
yellow
mass
of
flame burners. It is noticeable that,
the main contribution to the emitted
particles below
30
(proportional
nm
in diameter.
to the
mass
burners.
Bacharach for any of the three well
keep
seen
smaller than that of burner Y The total emitted
less, which is considered
requirements [8].
32
test
mass,
diameter under the
particle
be
diameter. The volume of
from the
the volume concentration
the three
particle
flame burner Y emits the
of the blue flame burner B stems from
Figure
the
mobility
mobility
the blue flame burner B lies between that of the two
due to the
to
can
"clean" combustion
mind, however, that in
adjusted
according
terms
of total
burners
to
yields
a
present legal
particle number,
4
Residential Oil Burners
there
still considerable amounts of ultrafine
are
the calculated total
particle
mass
of all
Total Number
Total Mass
ECO Fuel
ECO Fuel
[1/cm3]
[mg/cm3]
[1/cm3]
[mg/cm3]
Y
4.53-106
10.17-10"5
0.02-106
0.45 -10"5
Y-R
6.18-106
1.79-10"5
(no data)
(no data)
B
24.27-106
2.18-10"5
11.12-106
0.72-10"5
particle number and calculated total particle
investigated
(ECO).
constant
density of
significant
influence
a
1
of the
highly puri¬
is calculated from the size spectra,
mass
spherical particles with
assuming
g/cm3.
Variation of fuel
4.2.2
degree
particles.
of fuel
purity
The burners
In the
case
has
were
a
operated
with both
of the conventional
reduction of the number of emitted
yellow
particle diameters,
significantly (figure 7).
In the
case
depends
on
on
the number concentration of emitted
standard
quality
flame burner Y,
shape
purity
on
by
a
burner B,
weighted
both
fuel
with ECO oil leads to
magnitude throughout
of the spectrum is not altered
number and
operated with
the burner emissions is clear whilst its
flame burner Y
on a
highly purified
factor of at least two when
particle
produces
on a mass
magnitude
number and the calculated total
for all three burners and the two different types of fuel
yellow
operation
a
of the blue flame burner B, the difference in the emitted
the burner type. In table 4, the total
that the conventional
and
almost two orders of
while the
number is less dramatic, but still reduced
ECO oil. The influence of the oil
a
particles by
the whole spectrum of
mass
mass
burners Y Y-R, and B for standard fuel and
The
number and
summarized in table 4.
Total Mass
fied fuel
particle
are
Standard Fuel
three
a
investigated burners
particle
Total Number
Table 4. Total
(ECO).
emitted. The total
Standard Fuel
Burner
The
particles
even
are
particle
summarized. It is remarkable
less emissions than the blue flame
basis, when both burners
are
operated
with ECO fuel.
33
4
Residential Oil Burners
change
A
being
of oil has also
some
7.
Conventional
standard and
ECO oil,
Fuel additives
As
long
air-fuel ratio,
optimal
as
and may
[8]. This
in
means
particles
for
of the
particle spectrum,
of ECO oil
burner Y
the spectrum
(not displayed).
(Giersch), operated
oil. The solid line in the top
with both
graph
shows
respectively.
are
supposed
to
modern burners
only
shape
case
little soot is
conditions
increase
the
are
properly
produced
soot
that, in unfavorable
a
long
influence of additives
and the
emission
cases,
a
by catalyzing
maintained and
use
a
operated
of additives is
quite
of
Switzerland, for example, ask for
quite
-
reduce soot emissions
air-fuel ratio for oil burners is, however,
requirements
34
the
particles emitted with standard oil and those emitted with
Non-optimal burning
4.2.3
of
yellow flame
highly purified (ECO)
the ratio between
occur
on
shifted towards smaller diameters for the
Figure
C02.
influence
a
in
a
regime
of
optimal
not necessary.
The
critical. A reduction of this ratio
can
burner
usually
significantly [24; 28]. Legal
burner to be checked in intervals of 2 years
misadjusted burner
time before the next
the burnout of soot to
inspection
can
takes
emit immoderate amounts
place.
It may be of interest
4
Residential Oil Burners
whether, in
can
like this, the
a case
addition of small
prophylactic
quantities
of additives to the fuel
be beneficial.
In order to examine the influence of the fuel additive
flame burner Y
was
malfunctioning
or
maintained burner. As
badly
the BN
check-ups,
under
deliberately operated
measured
was
a
ferrocene, the conventional yellow
non-optimal
air-fuel conditions,
reference to
legally required
simulating
a
burner emission
for different concentrations of the fuel
simultaneously
additive.
First, the burner's air supply
reached in the
following
was
stationary operating
mode. The air
burner
Subsequently,
measurements.
concentrations of ferrocene additive, added to the
oil, cleaning and pre-burning procedures
experimental setup (section 4.1).
concentrations, the burner
4.5 had
stayed unchanged during
repeated
with ECO oil,
higher purity
of the fuel,
standard fuel led to the
Figures
same
of
Y
was
mentioned in the
with pure standard oil to
Except for
a
going
on.
change
emitted
verify
of
of the
that the BN of
33),
the
experiments
(due
were
to
the
with ECO fuel and
of number concentration, total number, and the
particles
as
function
a
conspicuous
seems
to
be
an
of
different
mean
ferrocene
additive
that the total number of emitted
particles
diameter
averaged mobility
adverse effect, the BN is nevertheless decreased
additives, implying that the
Figure
description
overall reduction of the BN
systematic
amount
of emitted soot is reduced
top axis). A plot of the emitted particle's volume concentration gives
what is
change
conclusions.
the former
upon introduction of
different
series of measurements with different additive
a
increases with the amount of added additive material while the
Although
three
the sequence of fuel variations. All measurements
concentrations in standard oil. It is
decreases.
with
standard fuel. After each
as
was
then left untouched for the
driven
was
original
section 4.2.2, page
see
8 and 9 show the
diameter
mobility
well.
as
After
BN of 4.5 with standard oil
a
supply
conducted
were
again operated
was
until
misadjusted
10 shows the volume concentration
as
a
more
(figure 9,
information about
function of the
mobility
diameter for different additive concentrations in standard oil. The main contributions to the
total
peak
particle
volume
maximum at about 100
the exhaust gas
the
(and hence
larger
are
trapped
on
the
nm.
Due to the
particle mass)
stem
experimental setup,
in the thermodesorber. The measured
size range, must be
become visible:
also to the total
one
composed mostly
hand, the
soot
of EC.
peak
at
from
most
large particles
volatile
compounds
particles, especially
Upon addition of additives,
100
nm
with
is reduced with
a
of
those in
two
effects
increasing
35
4
Residential Oil Burners
1.4x10
1
1.2
Additive Concentration:
-O- 0 ppm
-D- 6 ppm
1.0
-A- 15 ppm
-O- 22 ppm
0.8
0.6
0.4
0.2
i
i
i
Ti*hSP
,
10
100
Electrical
Figure
Number concentration of
8.
Diameter
Mobility
yellow flame
different concentrations of ferrocene additive
standard fuel
(0 ppm),
(d)
the burner has been
in
[nm]
burner Y
standard
misadjusted
to
a
operated with
fuel.
For
pure
BN of 4.5.
Bacharach Soot Number
BN 4.5
BN 4.4
7x10
BN 3.9
BN 3.5
35
~T
Total Cone.
6
Mean Diam.
[1/cm ]
[nm]
30
5
25
4
20
3
15
2
1
HI
=
10
0
0 ppm
6 ppm
15 ppm
Additive Concentration
Figure
9.
Total number concentration and
22 ppm
[ppm]
mean
mobility
diameter of
yellow
flame burner Y operated with different concentrations of ferrocene additive in
standard fuel. The measured BN
standard fuel
36
(0 ppm),
are
displayed
the burner has been
on
the top axis. For pure
misadjusted
to
a
BN of 4.5.
4
Residential Oil Burners
concentrations of the additive, i.e.,
oxidized. This leads to
maximum
at
about
a
are
in agreement with
doped fuels,
oxide
considerable amount of the emitted soot is
reduction of total emitted
25
concentration is raised,
a
is
nm
leading
mass.
On the other
to an
increase of total emitted
conducted
on
diesel
particle
engines,
where it has been shown that the small-sized additive
from the additive
particles stemming directly
i
Oil
2.0
i
peak
with
a
number. These
findings
also driven with ferrocene-
peak
consists
mainly
of iron
[29].
i
I
+
a new
formed, which is clearly increased when the additive
experiments
2.5x10
hand,
essentially
i
i
i
i
I
Soot Peak
Additive:
-O- Standard
+
0 ppm
-D- Standard
+
6 ppm
-A- Standard
+
15 ppm
-0- Standard
+
22 ppm
—
1.5
--a^--'--X^
1.0
Additive Peak
o
f)r/
Ü
0.5
O
>
0
i
i
i
10
10.
burner Y
Mobility
Diameter
Volume concentration of the emitted
(Giersch)
upon
to
a
(d)
[nm]
particles of yellow flame
operation with different concentrations of ferrocene
additive in standard fuel. For pure standard fuel
misadjusted
i
100
Electrical
Figure
i
(0 ppm),
the burner has been
BN of 4.5.
37
4
Residential Oil Burners
The reduction of soot
figure 11,
also be confirmed
can
by comparing
the absolute values of the measured PAS and DC
both the PAS and DC
normalized
signals
for the conducted
the active SA, calculated
by
the PAS and DC
signals
experiments
are
In
In
figure 12,
plotted again, however,
are
from the SMPS spectra.
displayed.
signals.
Comparison
of
figures
11
Bacharach Soot Number
BN 4.5
BN 4.4
BN 3.9
BN 3.5
8x10
E
CO
<
CL
O
Q
0 ppm
6 ppm
15 ppm
Additive Concentration
Figure
Absolute PAS
11.
concentration. The
DC
and
corresponding
For pure standard fuel
(0 ppm),
signal
BN values
22 ppm
[ppm]
as
are
a
function of the additive
displayed
the burner has been
on
the top axis.
misadjusted
to
a
BN of
4.5.
and 12 shows that the normalized DC
indicating
spectra
*
as
that the active SA, detected
expected
.
On the other
See section A. 6 in the
**
appendix
The ratio between the DC
signal
DC used for the
experiments
the DC, is correlated with the
on
underlying
SMPS
the calculation of the active SA.
and the calculated active SA in
a mean
in this
by
is constant within the accuracy of measurements,
hand, both the absolute and the normalized PAS signals
for details
accuracy of measurements and has
38
signal
figure
value of 3.8 instead of 1, due to
chapter.
an
12 is constant within the
arbitrary
calibration of the
are
4
Residential Oil Burners
clearly
reduced when the additive concentration is increased. This is
decrease of the aerosol's EC content
as a
an
indication for the
function of the additive concentration.
Bacharach Soot Number
BN 4.5
BN 4.4
BN 3.9
BN 3.5
PAS / Active Surface Area
DC / Active Surface Area
<
-
S
1
ü
Q
0 ppm
6 ppm
15 ppm
Additive Concentration
Figure
the
12.
PAS and DC
signal,
normalized
to
In
100
a
[ppm]
by
the calculated active SA from
respective SMPS spectra. The corresponding
the top axis. For pure standard fuel
(0 ppm),
22 ppm
BN values
displayed
are
the burner has been
on
misadjusted
BN of 4.5.
conclusion, the beneficial effect of the ferrocene additive, namely the reduction of the
nm
species
soot
of
peak
in the
particles,
case
most
of elevated emission levels, is
likely
iron oxide
case, the contribution of the additive
percent and
produces
additive
a
can
be
neglected.
significant
yellow
to
In table
flame burner Y,
with
a
the
size of 25
the total emitted
In terms of number
increase of the total
dosage (6 ppm).
conventional
peak
particles,
opposed by
mass
generation
nm.
In the
new
presented
is in the order of
a
few
concentration, however, the additive peak
particle concentration,
even
in the
case
5, the total number and calculated total
misadjusted
of a
to a BN
of 4.5,
are
of very low
mass
for the
summarized for two types
of fuel and various additive concentrations.
39
4
Residential Oil Burners
Additive
Total Number
Total Mass
Total Number
Total Mass
Concentration
Standard Fuel
Standard Fuel
ECO Fuel
ECO Fuel
[ppm]
[1/cm3]
[Lig/cm3]
[1/cm3]
[Lig/cm3]
0
2.23-107
11.39-10"4
1.34-107
7.16-10"4
6
3.10-107
8.91-10"4
2.50-107
5.93-10"4
15
4.42-107
8.23-10"4
3.79-107
4.91-10"4
22
5.23-107
6.85"
10"4
4.11-107
5.05-10"4
Table
Total
5.
conventional
number
particle
yellow flame
and
calculated
operation with different concentrations of
density of
1
a
to
a
of
mass
BN of
4.5, upon
ferrocene fuel additive. The
assuming spherical particles
with
the
mass
is
constant
a
g/cm3.
Conclusions
4.3
of the ultrafine
Comparison
has shown the
of
importance
particle
emissions of three
distinguishing
from the emitted total
emit
particles
high
amounts
spectrum (d
smaller
by
at
—>
6
of
At the
nm).
equipped
It is
at
common
of residential oil burners
of
particles
to
a
certain size
all three burners that
they
the small-sized end of the considered
side of the spectrum
{d
—>
220
nm), this number is
least two orders of magnitude.
The number of emitted
decreases
mass.
(106-107 cm"3)
large-sized
generations
the amount of emitted
(number concentration)
small
particle
(Giersch), misadjusted
burner Y
calculated from the size spectra,
total
clearly
with
a
with
for
a
increasing particle
widely-used
size. If the
conventional
yellow
yellow
10
nm) is slightly increased.
emitting
the
highest
amount
A blue flame oil burner is
of small
flame burner
flame burner is
FGR, the emission of most particle sizes is reduced, only the
particles (d <
in this respect,
particles
particles {d <
30
additionally
amount
even more
nm), but only
of very
extreme
very few
larger particles.
The conventional
yellow
contributions to the total
40
flame burner
mass
stemming
clearly
from
emits the
largest particle
larger-sized particles (d>
mass, the main
70
nm).
A FGR
4
Residential Oil Burners
added to the conventional
main
constituents in this
mass
produces
slightly higher
a
to note
very small
particles {d <
The influence of fuel
orders of
two
30
quality
is
yellow
less
flame burner
Addition
new
additive
of ferrocene
drop
even
to a
legal
limits
a
reduction of the
leads
that, due
particles.
peak produces
to a
far. For the
to
nm
a
soot
This beneficial effect is
mass.
of iron oxide
by
number of
yellow
flame burner
the whole size spectrum when
The emissions of the
below those of the blue flame burner,
quality effects,
additives
a
are
operated
particle
weighted
with ECO fuel. The
but the reduction of
particle
number concentration
case
a
of
a
bimodal
opposed by
number is
by
a
factor
well
4.5, where the
adjusted
in
burner
a
volume
particle
considerable reduction
the creation of
a new
25
nm
concentrations, the formation of the
increase of the total
BN of
of the
shape
peak, resulting
Even at low additive
significant
misruned burner with
apply
high
be achieved when ECO oil is used instead of standard EL oil.
of the emitted total
peak
The conventional
particles throughout
concentration. The additive reduces the 100
additive
flame burner. It is
of the very
mainly composed
basis, when both burners
on a mass
somewhat smaller. Nevertheless,
can
yellow
ECO oil instead of standard EL oil.
blue flame burner also features fuel
of at least two
is
The
The blue flame burner
large particles.
particularly striking.
magnitude
conventional
number and
mass
significantly.
nm).
highly purified
on a
still stem from
emission
mass
emission than the advanced
mass
driven with
both
case
that in this case, the
interesting
produces
flame burner decreases
yellow
particle
amount
(BN
lack of soot, the formation of small iron oxide
0.5
number. These
findings
of emitted soot exceeds the
or
less),
particles
it has to be
expected
upon usage of ferrocene
additives is the dominant effect.
41
5
Passenger
Vehicles
Passenger
5
The
large
ultrafine
two
amount
Vehicles
of passenger vehicles in the industrialized world is
in ambient air.
particles
Traditionally,
distinct types of internal combustion
diesel
•
For
a
when black clouds of soot
less
incentives
tax
European countries.
emissions
are
number and,
translates
still
on
diesel
From both
On
an
on a mass
a
a mass
engines:
(diesel engine),
With
the
particle
with maximum
The automotive
developing
low
industry
Despite
than those from
basis. The diesel
and economic
diesel
C02,
point
emissions
the
pipes
because
they
were
visible to the naked eye,
of passenger vehicles
motivated
by
diesel-powered
this
the diesel
.
engine's
passenger vehicles
a
conversion
the
fuel
a
of the two
and
particle
on
both
a
efficiency, however,
gas.
modern passenger vehicle
advantages
believes to have found
diesel
gasoline engines, weighted
(gasoline engine)
is even more
improvement,
principal greenhouse
of view,
fuel-to-energy
vehicles, this
even
engine's superior
gasoline direct-injection (GDI) engine.
heavy-duty
of
reputation
basis, today's modern diesel engines produce much
combustion of fossil fuels should combine the
combustion
bad
sometimes
high acceptance
into reduced emissions of
écologie
-
a
gasoline fuel,
versus
considerably higher
especially,
directly
powered by
engines)
emitted from the exhaust
were
emissions than older devices did.
particulate
Otto
vehicles had
of particulate matter
well known fuel economy, has led to
in many
of
engines (compression-ignition engines)
eject large quantities
Nevertheless,
source
engines:
long time, diesel-powered passenger
known to
major
the fleet of passenger vehicles is
gasoline engines (spark-ignition engines,
•
a
powered by
prevalent types
outstanding
of
fuel economy
efficiency.
solution to these
requirements by
Since 1997, automobiles
equipped
with
case
43
5
Passenger
a
GDI system
of
a
Vehicles
engine
GDI test
state-of-the-art
5.1
available
are
European market.
examined and
are
gasoline
the
on
compared
The extent to which
foremost
method of
on
preparing
internal combustion
an
brief
a
the emissions of
particulate
emissions
commercially available,
emissions
engine produces particulate
(EC)
the combustion strategy. The combustion strategy includes the formation
the air-fuel mixture, the type of
changed during engine operation.
process,
the
engine strategies
flame that results thereof. These parameters
be
chapter,
and diesel passenger vehicles.
Internal combustion
depends
to
In this
description
of the
For
a
usually
are
better
fixed
by
understanding
gasoline, diesel,
and the type of combustion
ignition,
the
engine design
of the
respective
and GDI combustion
and
can
not
combustion
is
strategies
given
below.
Conventional
formation of
homogeneous
engines inject
the
gasoline engines
the fuel
cylinder [30].
into the
air-delivering
compression stroke,
external
(i.e.,
use
a
outside of the
cylinder)
carburetor, while modern
inlet channel, close to the inlet valve of
the mixture is
bar, resulting in heating of the mixture
up to 30
by
air-fuel mixtures. Older models
directly
On the
characterized
are
to
a
typically compressed
temperature of 400
-
to pressures
500 °C. This
temperature is below the auto-ignition threshold. The air-fuel mixture therefore has
ignited by
a
flame. Well
spark [31].
prepared premixed
Diesel engines
heterogeneous
compressed
The type of flame that results from this process is that of
to
flames
characterized
are
produce only
internal
by
very small amounts of EC
(i.e.,
inside
formation of the air-fuel mixture. On the
a
pressure
The
(rurbocharged engines).
of 30-55
bar
a
particles.
compression stroke,
or
temperature of 700
be
premixed
cylinder)
(naturally aspired engines)
air reaches
compressed
of the
a
to
-
and thus
intake air is
bar
80-110
900 °C. This
temperature is sufficient for auto-ignition of fuel, injected into the cylinder shortly before the
end of the
compression
stroke. Fuel is
cylinder (indirect direct-injection, IDI)
fosters
than
diffusion-type
premixed flames,
achieve
44
a
injected
or
directly
either into
into the
improved mixing
mixing
of air and fuel
of air and fuel.
by injecting
prechamber adjacent
cylinder (DI) [31].
flame. Diffusion flames tend to emit
due to inferior
a
higher
Today's
fuel into the
amounts
the
This process
of EC
particles
advanced diesel
cylinder
to
engines
with very
high
5
Passenger
pressures,
Vehicles
independent
[31]). Injection
of
of fuel with
used for passenger
currently
GDI
engines
reduced amounts of fuel
the
process
cars are
hybrid engines
are
of air and fuel
mixing
1350 bar
injected directly
is enriched in order to
spark plug
throughout
are
the rest of the
engine operation
emissions
cylinder
charge (H)
to
high
reliable
ensure
S mode is
the GDI
In passenger vehicles
switching
into the air-filled
by stretching
while
a
between the
GDI
cylinder,
engines,
the
and H mode,
S
designated
is
a
a
The mixture
of air in the
low
NOx
in the
conventional
homogeneous-
gasoline engine:
fairly homogeneous
engine
and
on
mixture of
spark ignition.
electronics is
depending
and CO
flame.
operated
injection
regions
for low to medium
creating only
engine
and diesel
while the combustion
surplus
a
gasoline
spark plug.
diffusion-type
the time between fuel
powered by
pressures
stratified-charge (S) mode,
ignition,
The S mode is
consumption
requirements,
injected directly
air and fuel is attained
automatic
load
[30]. Injection
of the
vicinity
mode. The H mode resembles the features of
fuel is
although
and decreases fuel
In the
cylinder.
into the
injection.
that evaporate
higher [31].
or
is very lean, due to
[31]. The combustion flame of the
Upon medium
droplets
that share characteristics with both
further away from the location of fuel
load
for
common-rail system
quantity (e.g.,
very fine fuel
produces
pressure
required
fuel
injected
The air-fuel mixture is formed inside of the
engines.
near
high
and reduce the time
quickly
and
engine speed
the
responsible
for
respective driving
conditions.
5.2
Experimental details
The measurements considered here
performed
Due to
a
on
a
1-cylinder
GDI research
confidentiality agreement,
time. The
operating
are
conditions
are
emission measurements
engine
the exact
with
engine
jet-guided
(section 3.1,
page
mixture formation strategy.
data may not be disclosed at this
therefore referred to as, S
or
23),
H mode at low
or
point
in
high load,
respectively.
45
Passenger
5
Vehicles
Coulometric and
line with
gravimetric samples
dilution ratio of 1:8
a
dilution system,
provided by
system is extracted 1.7
24).
m
The SMPS system is
flow), leading
particle-free
to a
corrected for dilution.
at
temperature
no
nucleation
5.3
diesel
reason
engines.
capacity
of the
engine
In
S
are
is
for
one
high
the
on
-
sensors
and the SMPS
(point (A), figure 4,
Rotating
nm.
of
SmartSampler
1/min. sheath air
(3
650
particle
vs.
observed after
-
a
page
0.3 1/min. aerosol
disk dilution system and
condition of the
operating
exhaust
engine's
a
means
exhaust line
engine's
reaches values of 200
presented
engine,
data
are
the exhaust
700 °C. The thermodesorber is omitted since
test run.
homogeneous-charge
vs.
developing
GDI
To this
engines
engine
cylinder
power is low. At
volume and
more
the size spectra of emitted EC
mode
are
as
more
can
be
better than that of modern
as
described in section 5.1,
load conditions, however, where the full
pronounced.
to
In the H
more
particles
are
size stays the
required engine
power,
subsequent
resemble
a
und
for the S and H mode at
particle
same.
This
combustion.
emissions
can
be
are
elevated
explained by
the
By conditioning of the
diffusion flame, and the
generation
of
mode, better mixing of air and fuel reduces particle
similar to
a
premixed
opposed by considerably higher particle
Eidgenossische Materialprufungs-
compared
that in the S mode,
seen
particle
the combustion flame is
therefore
high
of
consumption
in the H mode.
load conditions. It
is
or even
fuel is needed to attain the
different modes of mixture formation and
particles
mode
is the effort to reduce fuel
end, the engine is operated in the S mode,
order of magnitude, while the
emissions
46
24) by
heated to 80 °C. The dilution factor is 1:300, the
mode, the combustion flame is likely
*
page
and to achieve fuel economy similar to
operated
figure 13,
same
soot
downstream of the
The exhaust gas for the
size resolution of 16
phenomena were
when the demanded
two
.
in low flow mode
Depending
point (A)
gasoline engines
by
operated
Stratified-charge
The main
the
EMPA
m
Results and discussion
5.3.1
the
(point (B), figure 4,
downstream of the
particle
dilution air
taken 1.5
are
Forschungsanstalt,
flame. Fuel
emissions.
CH-8600 Dubendorf
savings
in the S
5
Passenger
Vehicles
10°
'
I
E
;
10
q^q
;
10
UU
0/
-
;
Q
-_
_
-O- S Mode /
10J
High
High
-D- H Mode /
:
Load
W-^-t
Load
=
"
-
10'
10
100
Electrical
Figure
13.
in
S
the
Particle size distributions of
H
and
significantly
more
External
vs.
5.3.2
As described in section
gasoline
and GDI
gasoline engines
Mobility
engines
mode,
respectively.
1000
Diameter d
a
In
GDI
[nm]
engine, operated
the
S
and
particles while the particle size stays the
is the
cylinder,
more
difficult to achieve the
process of the air-fuel mixture. In conventional
preparation
The GDI
same
the time available between fuel
degree
place
and
factor is
formation.
Figure
operation
high
at
gasoline engine
14 shows
load. It
can
a
be
comparison
seen
the fuel
cylinder.
homogeneity
mainly
the
that
mixture is formed
directly
into the air-
This method makes it
can
be
mixing time,
accomplished
determined
strategy, the GDI research engine is
with external and thus
premixed
air-fuel mixture
of the two mixture formation modes for
that external mixture formation leads to
a more
combustion, since the number of emitted EC particles is notedly smaller than in the
of fuel into the air-filled
by
spark ignition.
In order to examine the effects of the mixture formation
conventional
homogeneous
inside the
of air-fuel
limiting
injection
a
engine, however, injects
of air and fuel takes
with external mixture formation. The
as a
same.
5.1, the conceptual change in engine design between conventional
filled
operated
load
internal mixture formation
cylinder.
mixing
high
mode, the engine emits
with external air-fuel mixture formation,
before it is led into the
at
engine
complete
case
of DI
cylinder.
47
5
Passenger
Vehicles
Figure
14.
Internal
vs.
external mixture formation
mixture formation leads to
better air-fuel
a
on a
homogeneity
GDI
engine.
External
and reduces
particle
emissions.
order to get
In
conventional
against
an
and
of how
test
high
as a
bench that is
load H
being compared
operating points
measurements
to
engine performs
size spectra of the GDI
GDI
emissions of
operated
a
GDI
closer to the diesel
a
in the S mode.
engine
on
plotted
in
15
lie between those of
engine.
a
in
comparison
engine
a
(a)
plotted
comparison
1-cylinder engine
The low load S
at
speeds
of 50 km/h and
with the GDI
engine
are
15.
under low load conditions is most
indicates that, in this case, the
conventional
The total number of emitted
smaller than the total number of emitted diesel
a
are
to
in round terms to constant
comparison
figure
is
dynamometer.
dynamometer
engine running
Figure
on a
engine
engine correspond
passenger vehicles used for
For the sake of fuel economy,
be
vehicles tested
of passenger vehicles
are
to
since the GDI research
of the GDI
listed in table 6, the size distributions
48
GDI
engines, particle
rough estimate,
km/h, respectively. The
likely
the
those obtained from modern, state-of-the-art passenger vehicles. This
velocity
120
impression
and diesel
gasoline
should be understood
on a
to state-of-the-art passenger vehicles
Comparison
5.3.3
gasoline
particles
engine particles by
a
and diesel
particle
engine,
from the GDI
but
engine
is
factor of about four. Note
5
Passenger
Vehicles
Year of
Label
Engine Type
Vehicle
G1
Gasoline
Audi A4 20V
G2
Gasoline
D1
Diesel, DI
D2
Diesel, IDI
1997
125/5800
1990
75/5200
Audi A4 1.9 TDI
1997
110/4150
Citroen BX 19 TZD
1994
90/4300
Opel
performed
are
on
[PS]
atRPM
Table 6. Vehicles used for
ments
Power
Manufacture
a
Kadett E 1.6
comparison of particulate emissions. Measure¬
dynamometer
at constant velocities of 50 km/h
and 120 km/h.
that the
particle
engine.
This may be related to the fact that DI and D2 have two different types of
vs.
size distribution of vehicle D2 differs
IDI). Compared
emitted
by
the GDI
to
engine
section 5.3.1, the fuel
amounts
In
lie
of emitted
high
quite
load
savings
achieved
by
Gl and
magnitude higher.
the S mode
are
from that of DI
or
the GDI
engines (DI
G2, the number of particles
As
was
already
mentioned in
opposed by significantly higher
particles.
15
in between those of the
gasoline engines
gasoline engines
is two orders of
operation, figure
number of emitted
engines
the conventional
remarkably
particles
(b),
the
particulate
gasoline
from the GDI
engine
is about 30.
the size distribution of the GDI
engine
engine
in H mode
and diesel vehicles. The ratio between the total
engine
and those emitted from the conventional
Gl and G2 is about 75. The total
and the GDI
emissions of the GDI
Apart
particle
number ratio between the diesel
from the difference in number concentration,
and the diesel
engines
look
quite
similar.
49
5
Passenger
Figure
15.
Vehicles
Comparison of
(D1, D2, G1,
vehicles
and
the GDI
G2)
engine
defined in table 6.
are
in the S mode and the vehicles maintain
engine
is
operated
Validation of
As described in section
(total mass)
employed.
(DC)
In the
for
conditions.
sensor
are
(b)
120
the
At
is
operated
the GDI
high load,
km/h,
and OC
mass)
The
advantage
analysis
were
constant
also examined with
methods. In addition,
of the
of transient
sensors
one
in
PAS and
velocity.
second and their
sensor
engines
a
DC
to
filter
were
sampling
simple handling,
of combustion
operating cycles
emissions of combustion
gravimetric
and to the active SA
comparison
demonstrate the correlation between
particulate
a
chemistry (PAS)
and coulometric data, and SMPS data. This proves the
evaluating
engine
The
measurements
time resolution of down to
we
50 km/h.
conditions
sensitive to the surface
them to be used for the
gravimetric
50
high
following sections,
sensors
(EC
particles.
methods lies in their
velocity of
driving
dynamometer.
a
At low load, the GDI
5.2, the GDI engine emissions
sensors are
of combustion
enabling
constant
(a)
on
kindly provided by [34].
particle
and coulometric
These
a
in the H mode. The vehicle
Measured passenger vehicle data
5.3.4
with passenger vehicles
engines.
data, conventional
applicability
under various
of these
operating
5
Passenger
Vehicles
Comparison:
5.3.4.1
Measurements
of EC, measured
consist
into
roughly
performed
diesel
by means
a
diesel
vs.
engines
PAS. In the
a
case
engines
show that the PAS
of coulometric
of EC. EC has
mostly
detection with
on
GDI
analysis [32; 33].
high photoelectric yield
of diesel exhaust,
0.1 |lg of EC per cubic meter of
with the GDI
engines. Figure
engine
are
in very
16 shows that the PAS
a
correlates well with the amount
signal
PAS
sampled
Fresh aerosols from diesel
and is therefore well suited for
of 1 fA
signal
air
typically
[32; 34]. The
good agreement
translates
measurements
with the results from diesel
correlates well with the EC content
signal
engines
over
the
whole range of measurements.
3
0x105
I
I
I
Linear Fit
----
1 fA
•
=
0 11
jig/m3
EC
a''
,1"'
20
§)
I
Measured Data
•
25
I
,-'
1 5
CO
y
,--'''•
CL
1 0
05
R2
9 0859
=
0 9748
*
x +
3626 1
-
V
0
C)
i
i
i
I
I
05
10
15
20
25
16.
determined
correspond
Correlation between PAS
by
coulometric
signal
and EC
mass
analysis of filter samples.
to variations of the GDI
3 0>
104
[jig/m3]
EC
Figure
=
engine's operating
concentration,
The
data
points
conditions.
51
5
Passenger
Vehicles
Experience
with the
with diesel
total
particle
measures
requires
do not
conditions
are
engine,
change substantially.
often
PAS
whole range of
sufficiently
calculated
fulfilled.
from the
SMPS
and that the chemical surface
With combustion
particle
particles
17 shows
Again, figure
and calculated total
signal
as
correlates well
signal usually
that the relative EC fraction remains
varying engine operating conditions,
particles
GDI
has also shown that the PAS
concentration,
mass
correlation of these two
upon
engines
mass
spectra. The
fairly
constant
properties
from diesel
of the
these
engines,
that, also in the
case
concentration correlate well
of the
over
experiments.
3
0x105
i
i
l
l
I
l
Measured Data
•
25
l
Linear Fit
20
•
§)
1 5
CO
•
CL
1 0
----''
6938
y=1
R2
05
»w
0
=
17.
i
i
i
I
I
I
0 04
0 06
0 08
0 10
0 12
014
Correlation between PAS
(rough)
the counted
engine's operating
calculation of the total
particles
are
signal
[jxg/cm ]
and total
mass
52
for all
particles
concentration,
particle
mass
spherically symmetric
that
are
detected
by
to
conditions.
from the SMPS spectra
and have
a mean
Furthermore, the SMPS spectra should be complete in the
account
0 16
3
respective SMPS spectra. The data points correspond
variations of the GDI
The
19196 1
i
calculated from the
*
+
0 02
Calculated Total Mass Concentration
Figure
106*x
0 95522
the PAS.
assumes
density
sense
that
of 1
they
that
g/cm
.
should
the
5
Passenger
Vehicles
Total active surface
5.3.4.2
As mentioned in section 3.1.4
and
can
be calibrated to
has been done for the
yield
area
(page 25),
the total active SA,
experiments
the GDI
on
calculated total active SA shows that both
since the
slope
of the linear fit in
6x105
figure
i
•
5
—
the DC
is
signal
as
proportional
18 deviates
i
the total active SA
calculated from the SMPS spectra. This
engine. Comparison
quantities
to
are
only
of the DC
related within
signal
and the
acceptable variations,
little from the theoretical value of 1.0.
l
l
l
Measured Data
•
Linear Fit
•-''
CO
4
E
•.-'-'
•
e*
E
r*'
S
i
3
ro
c
#
CO
Ü
y
2
Q
J
.%
n
tr
C)
\
+
M
1
-'-'" \
y=1
R2
P
I
I
12
=
1076*x +21917 1
0 9637
I
I
I
3
4
5
Calculated Active Surface Area
Figure
18.
Correlation between DC
signal
[jim
2
/cm
3
6x
o5
]
and total active
SA, calculated
from the respective SMPS spectra. The data points correspond to variations
of the GDI
engine's operating
conditions.
53
5
Passenger
5.3.4.3
In
Vehicles
Total
figure 19,
determined
the total
particle
long
as
the material
It is
expected
deposited
on
the
stressed, and the corresponding size distributions
measured
operated
on
special
(Exp.
case
Figure
operating
013 and
have
Correlation
experiments.
that
the
not
The data
inset
especially
displayed
those
the total mass,
be
can
is
operated
three
points
in the inset. Most
points
In
figure 19,
Exp. 024, where the engine is
points
with very different size
as a
conventional
shows
the
particle
to variations of the GDI
size
distributions
points.
In
gasoline engine
particle number concentration and total
points correspond
as
completely
correlate well with the other measured
engine
between total
The
are
filters
nm).
size distribution similar to
seems
points,
by gravimetry.
conditions.
a
Exp. 015) do
of these two
19.
determined
54
engine
in the DI S mode. It
distributions
the
the GDI
650
-
mass
correlation between these two
a
gravimetric
(16
total
plotted against
that there is
accounted for in the available size range of the SMPS
are
gravimetric
vs.
number concentration is
by gravimetric analysis.
as
measures,
particle number concentration
of
mass,
engine's
selected
5
Passenger
Vehicles
with external
preparation
respectively).
While it is
gravimetry
operating
The
a
conditions of the
investigation
engine
are
responsible
In the S
be
mode,
GDI
a
concerning
large
a
explained by
the mixture is rich
condition leads to
requires
a
a
engine,
a
the EC
from either the SMPS system
errors
that the
likely
more
for the observed
or
different
fundamentally
discrepancies.
of EC
the
amount
by
a
is
into the
gasoline engines
with
cylinder.
produced, compared
to
relatively heterogeneous
produces
increasing
more
soot
than
DI of fuel into the
cylinder
homogeneous
and
the H mode. This
mixture is
ignited;
distance thereof. This
a
premixed
flame. The
approximated
in the H
subsequent mixing
with air,
of the air-fuel mixture and is better
of soot than the
has shown that there
engine
formation between
injected directly
particles
flame that
diffusion-type
GDI research
and very lean with
spark plug
good homogeneity
higher
(soot)
the fact that in the S mode,
near
a
where air-fuel mixture formation is realized in the
where fuel is
amount
mode. The H mode, defined
produces
from
particles
(external) injection systems,
inlet channel, and
latter
sampling
of the data, it is
of combustion
difference
significant
conventional
can
scattering
cause some
that
possible
and 0.8,
(1.3
Conclusions
5.4
is
of the air-fuel mixture and different air-fuel ratios
condition realized
by
external mixture
formation in the inlet channel.
A
rough comparison
appropriate driving
modes
emitted from the GDI
gasoline
of the GDI
(S
at
engine
low load, H at
produces
less than passenger vehicles
produces notedly
same
degree
of
particles
and diesel passenger vehicles in the
high load)
high
expected
gasoline
amount
equipped
particles
homogeneity
gasoline engines.
more
less
a
be
can
combines features of both conventional
S mode
gasoline
shows that the amount of
lies somewhere in between the
engine
and diesel vehicles. This
fuel-saving
with
to some
and diesel
corresponding
degree,
engines.
emissions from
since the GDI
engine
It should be noted that the
of particles, estimated to
with modern diesel
particles
only
about
engines. Although
a
factor four
the H mode
than the S mode, the mixture of air and fuel does not attain the
as
in the
case
For this reason, the GDI
in the H mode than
a
of external mixture formation in conventional
engine produces
comparable
conventional
at
least
one
order of
magnitude
gasoline engine.
55
Finally,
of
a
the
comparison
PAS and
particulate
down to
a
DC has proven the
emissions of combustion
one
applicability
engines.
second which makes them
operating cycles
56
of gravimetric, coulometric, and SMPS data with the
of
engines.
The
of these
sensors
especially
sensors
feature
a
attractive for
sensor
signals
for evaluation of the
high
time resolution of
investigating
transient
6
Working
6
Area Measurements
Area Measurements
Working
The
of
use
heavy-duty
sites
in
tunnels
Environments like these
many
engines
concentrations
particularly high
construction
diesel
are a
in environments with insufficient ventilation leads to
of emitted combustion
and
closed
mines,
constant
challenge
threshold limit values for the amount of foreign
areas are
being tightened.
fraction of airborne combustion
For the
reasons
role, since EC is
In this
chapter,
a
we
selected
measurements are
6.1
areas
compared
where
to
occupational
areas.
health. In
mandatory
per unit volume of ambient air at
mass
of this
(page 21),
development,
the
the detection of EC
particles originating
present photoelectric charging
working
covered
are
respirable
ultrafine
is in the center of interest.
reliable tracer of airborne
particulate
other
for the surveillance of
particle
course
mentioned in section 2.6
field measurements of the
two
In the
particles
and
buildings
health is treated with great concern, and
developed countries, occupational
working
particles. Typical examples
as a
simple
EC concentration in
occupational
plays
an
important
from combustion processes.
and online method for continuous
air, stemming from diesel exhaust,
at
health is at risk. The results from two field
laboratory experiments
under well controlled conditions.
Online detection of elemental carbon
Particles
from
diesel
emissions
engine
contain
mostly
EC.
Coulometry [26]
is
a
conventional and standardized method for determination of the EC content in air. Filter
analysis
methods like
coulometry
integral
value
certain time
over a
have several
period,
the
disadvantages:
sampling
the obtained results represent
times for sufficient filter
loading
an
are
57
and the
usually quite long,
makes the whole process time
consuming
It has been shown in many
there is
a
detected
good
by
and
with
experiments
of coulometric filter
means
particle
permitting
particles
The
Bitburger brewery
in
purpose of unloading empty
trucks
(model
goods
are
goods
organized
reduced number of
performed
the indoor
meets
brought
with respect to the
areas
loading
leaving
day-time
stem
ventilation system, based
motivated
increasing steadily
particle filters,
loading
ventilation system.
onto
in three shifts
block storages that
in two shifts per
area are
mostly
the
goods
and
an
are
by
loading
for the
area
diesel trucks. These tasks
means
with soot
situated
of diesel fork-lift
particle filters).
of the
sideways
additional shift at
The
loading
night-time
with
a
employees.
with soot
area
full
indoor
an
lifting capacity, equipped
to
measurements are
loading
loading
employees
70
the demands with respect to
equipped
and
perform
Bitburger brewery, Germany
from and
Linde H 80 D, 8 tons
taken from and
Work is
The
this fact, the
to
emitted from diesel combustion
working
Bitburg, Germany, operates
performed by approximately
area.
as
Motivation and purpose of the measurements
6.2.1
are
that
in air.
Field measurement 1:
6.2
58
particles
5.3.4]. Owing
second. A PAS enables to
one
constant, automatic, and time-resolved surveillance of
concentration of ultrafine EC
engines
PAS and the EC content,
a
section
analysis [32; 33;
time resolution of down to
a
laboratories which
emissions from diesel
from
signal
of ultrafine EC
monitoring
specially equipped
expensive.
correlation between the measured
PAS is suitable for online
processes,
has to be done in
analysis
working
on
only.
the fact that the diesel soot emissions inside
and the
area
air
existing
ventilation system
quality. Though
no
longer
the fork-lift trucks
are
it is assumed that the diesel soot emissions inside the
from them because
area
by
The
they operate
brewery
insights resulting
is
much
planning
more
to
than the trucks
install
from measurements
a new
performed
entering
and efficient
on
the
existing
6
Working
Area Measurements
Experimental
6.2.2
details
The measurements considered here
The indoor
can
be
operated
h fresh air
are
loading
6.2.2.1
30
is
and 6700
(breadth),
Test
m
run
m
(model
/h exhaust air
VRG710).
LTG
only,
page
27).
Each ventilator
combined 5300
or as a
The dimensions of the
supplies only.
only
-
12
m
m
/
loading
area
325
are
m
(height).
12 exhaust air ventilators of the first half of the
power), leading
additional air is
supplied by
flow of 120'000
m
means
ventilators
(section 3.2,
measurements
1: ventilation at half power
% ventilation
This setup leads to
area
/h exhaust air ventilator with heat recovery. The block storages
and 10
For this measurement,
operated (50
equipped with 48
with fresh air
m
working
either for removal of 12'800
supply
equipped
(length),
area
are
12
ceiling
away 150'000
air
exchange
of coulometric filter
analysis
are
loading
area
of 2.6/h. Both online PAS
rate
area are
/h of exhaust air. The necessary
ventilators in the block storage which
/h. The additional air enters the indoor
an
m
loading
provide
mainly
signal
near
a
volume
floor level.
and EC content
measured in the centre of the first half of the
by
loading
area.
6.2.2.2
Test
run
2: ventilation at full power
For this measurement, all 24 exhaust air ventilators of the first half of the
operated (100
% ventilation
lack of fresh air
an
to
the first test
open door in the block storage
first half of the
5.3/h.
are
compared
power), leading
Again,
loading
area
(15'000
(43'000
both online PAS
signal
away
run
m
m3/h).
is,
/h)
a
total of 300'000
among other
and
a
m
measured in the centre of the first half of the
/h of exhaust air. The
partially opened gate
by
loading
area are
things, additionally supplied by
This arrangement leads to
and EC content
loading
means
an
in the middle of the
air
exchange
of coulometric filter
rate
of
sampling
area.
59
Evaluation of the ventilation
6.2.3
From the first two test runs,
coulometry)
a
conversion factor between PAS
is obtained. The PAS
signal
can now
concentration. With this information, it is
locations inside the indoor
corresponding
performance
inside the
ceiling
in the whole
loading
level
loading
EC concentration.
area
Thus,
loading
area are
system
be translated
possible
to
signal
directly
perform
resolved
spatially
area can
into the
mean
PAS
block
block
block
storage 2
sto. 3
I
/
offices
block
block
storage 4
storage
5
MP8
',
MP9
I
trucks
-A
~"
I
offices
door used for ventilation
indoor I oading area, first half
Figure
20. Ground
indoor
loading area,
plan (schematic) of the indoor loading
second half
area
and the block
storages of the Bitburger brewery. The points denominated MP indicate the
locations where air
60
quality
into the
taken both at floor and at
MP10
MP7
different
of the ventilation system
analysis
measurements are
storage 1
MP6
EC
be undertaken. Different measurement locations
examined, whereby
entry
at
signal
(figure 20).
trucks
(from
respective
measurements
with the PAS and convert the
a
and EC content
measurements
are
performed.
6
Working
Area Measurements
6.2.4
Results and discussion
Figure
21 shows the online
determined
full power
Comparison
leads to
a
runs
of the
1 and
mean
The
amount
diesel
measurements on
sampling
figure
loading
of EC
mass
21
are
a
of
one
as
air.
sampled
mean
determined
good agreement
measured data that the EC concentration in
and
a
by
half and two hours.
means
For better
of
coulometry,
comparison,
is
proportional
section
by coulometry [32; 33;
with these
mg/m
signal
PAS
,
as
findings.
determined
the
to
the
5.3.4].
It follows from the
by
coulometric filter
50% ventilation
2000
x104 (integral)
•EC
PAS
c
as
factor of lO'OOO. It has been shown in various
emissions that the
in
EC value
area, for ventilation at half and
time lies between
m
per
multiplied by
engine
respective
be used to translate the measured PAS current into the
can
value of the EC concentration
The results from
with the
PAS value with the EC content, determined
coulometric EC value is
integral
2).
conversion factor that
corresponding
together
inside the first half of the
by coulometry
(test
of the PAS,
signal
(online signal)
1500
O)
CO
CO
<
^
1000
E
-
E
irfdfïwr
500
X
irVtftf f*%mf
100% ventilation
O
>EC
LU
x104 (integral)
-PAS
00:00
Figure
21.
concentrations
00:30
Measurement
01:00
of
(horizontal lines),
at half and full power. For better
the
as
01:30
Elapsed
Time
online
PAS
measured
by
(online signal)
02:00
[hh:mm]
signal
and
the
coulometric filter
comparison, the EC values
are
corresponding
analysis, for
EC
ventilation
multiplied by 104.
61
analysis,
can
be derived from the online PAS
This conversion is used to evaluate the EC concentration
lO'OOO.
measurements
Figure
loading
the
signal by dividing
with the PAS
sensor
at
different locations inside the
by
loading
be
point.
signal by
of online
means
area.
22 shows the results of various PAS measurements at different locations inside the
area.
At each
presented measuring point (MP),
the online PAS
is recorded for 10
signal
minutes. With the conversion factor obtained from the first two test runs, the
can
PAS
mean
translated into the EC concentration in
directly
This has been done for the data
presented
in
figure
mg/m
the
at
mean
signal
respective measuring
22.
0 35
online PAS
MP
PAS
mean
7, ceiling
PAS
signal
signal
0 30
0 25
legal
E
0 20
ü
015
MP
EC limit 0 1
mg/m'
6, ceiling
MP
10, ceiling
0 10
0 05
MP
6, floor
0
00 00
00 15
00 30
00 45
Elapsed
Figure
area.
of
22.
The PAS
mg/m3.
m3
at
Online and
signal
mean
PAS
signal
Time
The horizontal solid line indicates the
working
areas
according
to
concentration at
ceiling
level is
0115
0130
0145
[hh mm]
at different locations inside the indoor
has been converted into the
corresponding EC
mandatory
loading
concentration in units
threshold limit value of 0.1
mg/
[35].
MP 6 is located in the first half of the
roughly
loading
double
of three factors. First, the fresh air enters
62
0100
near
as
area, close to
high
as
at
one
of the ventilators. The EC
floor level. This is
a
consequence
the floor level. Second, the fork-lift trucks emit
6
Working
Area Measurements
their exhaust gas
upwardly. Third,
the hot exhaust gases
driven to the
are
due to
ceiling
convection.
MP 7 is also located in the first half of the
segment of the ceiling without
same as
a
ceiling level, however,
the fact that there is
is three times
floor level. This
can
measuring point.
The exhaust gases accumulate in this segment of the
explained by
MP 9 is situated in the second half of the
ventilators
are
driven in exhaust air mode
in the mixed fresh air / exhaust air
emitted
through
the
level is
higher by
ceiling.
0.025
,
in
concentration is lower
by
0.150
MP 10 is located in
an
adjacent
at
loading
only,
low EC
mixing
comparison
mg/m
,
in
to MP 6. At
comparison
These data have
loading
area
clearly
that it is necessary to
indoor
loading
in the
sense
anywhere
a
perform
in order to
that the
inside the
data,
suitable than
a
a
ensure
air
loading
area.
mixing
In
a new
particular,
supply
operated
collected and
are
the EC
loading
area.
from the
There
ceiling.
was no
traffic
This results in
the
a
EC
effect that emissions settle to the floor
existing
design
ventilation system within the
of
measurements at
a new
system. They show
various locations
ventilation system
can
be
across
the
designed properly,
are
not
exceeded
the measurements have shown that in this case,
from floor level and air extraction at the
ceiling
seems
mode ventilation strategy. Due to the online character of the PAS
The EC concentration inside the
the amount of trucks
permanently
are
ceiling level, however,
values for the EC concentration
fast assessment of the EC concentration
on
an
moreover, the
necessary, continuous surveillance of the air
i.e.,
the first half, where all
level. At floor level, however,
ceiling
quality
that
required limiting
ventilation strategy with air
more
supplied
assisted the evaluation of the
Bitburger brewery and,
area
to
from above.
greatly
of the
ceiling.
to MP 6.
hall to the first part of the
concentration at
supplied
opposed
ventilator close to this
mode condition, the EC concentration at floor
concentration is elevated. This may be related to
while fresh air is
a
than at
higher
the ventilators in the second half
the time of measurement. In this hall, fresh air is
comparatively
As
area.
ceiling
no
mode, where both fresh air and exhaust air
Under the
mg/m
6, it lies in
In contrast to MP
area.
ventilator. The EC concentration at floor level is about the
for MP 6. The EC concentration at
be
loading
being
installed PAS could
loading
throughout the
quality
area
loading
area
is feasible. If
possible.
obviously depends
loaded at the
provide
is
whole
same
data for the
on
the amount of traffic,
time. It is worth
steering
mentioning
unit of the
new
that
a
ventilation
63
system, allowing
to
adjust
the ventilation power
automatically according
to
the momentary air
contamination.
Field measurement 2: Railroad tunnel construction
6.3
site, Switzerland
Motivation and purpose of the measurements
6.3.1
The Swiss Federal
Railways (SBB)
order to cope with the
purpose of
evaluating
measurements
with
growing
the
constructing
a new
tunnel in Thalwil
volume of traffic to and from the
working
emphasis
are
area
conditions in
a
Zurich in
of Zurich. For the
city
tunnel construction site, air
the EC concentration
on
near
performed
are
quality
inside the
tunnel
construction site.
Experimental
6.3.2
details
The measurements considered here
An online PAS is
placed
inside the tunnel
are
ventilated
by
means
next to a
taken in
are
working
area
measurements
coulometry sampling point
hourly
where filter
intervals. The tunnel has
of three air tubes with
a
a
diameter of 180 cm,
length
a
velocity
While the
in two
of 1.06 m/s. Work is
highest particle
sidewing
emissions
organized
page
27).
samples
of the air
of 4600
m
transporting
fresh air per second into the tunnel. The exhaust air flows back outside
with
(section 3.2,
through
18
-
60
and is
m
of
the main tunnel
in two shifts between 06:00 and 22:00 o'clock.
obviously
occur
at
the main construction
tunnels that lead away from the main tunnel, the PAS and
points, namely
coulometry samples
are
taken in the main tunnel closer to the tunnel exit in order to examine the contamination of
the
backflowing
air.
Tunnel construction consists of
emissions from
filled with
treatments.
64
a
heavy-duty drilling
lot of other
The
a
foreign
humidity,
in
multitude of different
machines and
matter
general,
like dust
worksteps. Among
transporting trucks,
resulting
from
particle
the tunnel air is also
blasting
is elevated inside the tunnel.
diesel
events
and shotcrete
6
Working
6.3.3
Area Measurements
Results and discussion
Figure
23 shows the measured online PAS
the tunnel. The
big
The
measurement.
fluctuations
integral
with the
mg/m ).
It is visible that the
In the
case
due to the different
concentration,
as
mandatory
measured
of the last measurement
limit value is
cycle,
for
figure
inside
good
tunnel construction site, there is
a
clearly
example,
exceeds the threshold limit value. From
a
worksteps performed
by coulometry,
allowed threshold limit value of EC for diesel
together
legally
EC
are
for selected measurement intervals inside
signal
24 it
even
can
engine
be
integral
seen
the
is also
exceeded at certain
the
on
day
of
displayed,
emissions
points
(0.1
in time.
coulometric EC value
that, also for the aerosols
correlation between the PAS
signal
and the EC
2000
PAS
O
EC
(online signal)
(integral)
legal
EC limit
lOOng/nV
1500
g
"S
g>
1000
w
w
<
Q.
500
0
1—1
o
o
oo
coo
oo
coo
oo
coo
oo
coo
oo
coo
OO
COO
OO
coo
o
o
0)0
mo
0)0
mo
0)0
mo
0)0
mo
0)0
mo
ct>oo
inco
0)in
CM
CNICO
COM"
M-m
in cd
CDI^
1^00
COO)
Time
Figure
23.
Measurement
concentrations
(rhombs),
as
of
the
[hh
by
ss]
PAS
online
determined
mm
at
concentration,
working
as
areas
measured
according
to
signal
and
coulometric filter
construction site. The horizontal line indicates the
mg/m3
in^t
mandatory
the
corresponding
analysis,
EC
inside the tunnel
threshold limit value of 0.1
[36].
by coulometry.
It
is, therefore, again possible
to
calculate
a
65
conversion factor for the PAS,
EC
to
concentration. In the
mass
the
respective
EC
mass
allowing
to
presented
translate the PAS
case,
signal directly
division of the PAS
a
concentration in units of
|lg/m
into the
signal by
respective
7 leads
directly
.
1800-p
1600-
1400--
Ü
1200-
i
1000-
w
CO
£
Linear correlation
800coefficient
c
®
R2
=
0 9780
600-
400-
200-
00
50
100
150
EC
Figure
measured
6.4
Correlation between
24.
by
means
Laboratory
200
[jig/m3]
PAS
mean
of coulometric filter
signal
and the EC concentration,
analysis.
measurement:
graphite particles
The field measurements have shown that, in both cases, there is
signal
factor
of PAS and the EC
depends
is conserved
on
over a
concentration
can
mass
the type and
where the
be varied
content,
origin
wide range of
laboratory experiments,
66
as
Motivation and purpose of the measurements
6.4.1
the
250
as
measured
good
by coulometry.
correlation between
While the conversion
of the aerosol, the correlation between the two
particle
to
measures
concentrations. This property is also confirmed in
particle composition
according
a
requirements.
is better known and where the
particle
6
Working
Area Measurements
Experimental
6.4.2
Carbon
in the nanometer size range
particles
with
discharge particle generator
nitrogen
graphite
are
electrodes. The
is extracted
particles
by
of
means
a
different number concentrations of carbon
doing,
equipment
while the
The carbon
the
This
produced by
particles
gas flow in order to minimize contamination of the
of the carbon
count
details
size stays
particle
particles
fed in
are
particles according
experimental arrangement
with respect to the
formed and carried in
disk dilution system
rotating
particles
be fed into the
can
spark
a
surface. A certain fraction
particle
parallel
into
serves
a
PAS and
mobility
a
SMPS, in order
[22].
In
so
measuring
to
classify
and
diameter.
First, the linearity of the PAS signal
two purposes.
concentration is verified. Second, the
particle
are
Palas GFG-1000
unchanged.
their electrical
to
a
long-term stability
of the PAS
is examined.
6.4.3
In
Results and discussion
order to
examine
concentration of
into the
carbon
sensor
signal
by
The
of
means
linearity
shape
of
a
of the PAS
Measurements with carbon
particle
size
a
In order to examine the
average
value
are
same as
is
plotted
in
usually
figure
over a
size spectrum is also
signal
as
particles
a
are
function of
the
significant
figure 26,
period
both
influence
and
in the range of
some
on
and
ten
plotted
numerous
particle
linearity
days.
of the
a
fed
diameter of the
figure 25,
function of the
values of the PAS
shape
sizes
(shift
good.
of the
signals.
of the PAS,
a
defined size
The constancy of number
of the size spectrum
reproducibility
as
are
number concentration is
long-term stability
shape
mean
the
on
mobility
particles
displayed (inset).
particle
of six months. The
25. The measurement
are
number
particle
with the SMPS system. In
conducted with various
reproducibility
time
parallel
typical
mobility diameter,
with the SMPS system. In
in
and electrical
number concentration
spectrum of carbon particles is generated
concentration,
with respect to
PAS
Shape
regularly
particle
This has
spectrum).
dilution unit.
checked
are
and the total
dilution ratio. The
of the
linearity
defined aerosol, various number concentrations of carbon
a
particle spectrum
the PAS
the
signal
of the
are
regularly
and the overall
particle
of most aerosol
verified
mean
distribution is the
measuring techniques
percent. In comparison, the presented result is quite
67
6
Working
Area Measurements
1200
1 2x10
]
[1/cm
1000
800
Concetraion
Number
w Ul o
o J\
.
w Oo
N) Ul o
N) O o
-* Ul o
-* O o
Ul o
ii
Average
10
Electrical
Mobility
Diameter
=
Signal [fA]
PAS
•
28 5
nm
[1/cm3]
SMPS
1 0
>*"£
08
100
Diamter
4=
c
CD
O
c
o
[nm]
600
O)
0 9986
=
R2
W
06
0
=
9919^
O
CD
<
CL
400
-
04
Q.
200
02
o
Linear
—i
1
05
1—
10
15
100
Figure
25.
PAS
signal
x
\
1
1
20
25
30
and total number concentration of carbon
diameter of 28.5
35
Dilutionratio
the dilution ratio. The inset shows the associated
mobility
Regression
particles
as a
particle size spectrum with
function of
an
average
nm.
1200
•
1000
£
_
--•
•
#
•
•»••••••
•
w
• •
•
v«
_
«
-
••,«-
800
"rö
ö)
600
Daily Average PAS Signal [fA]
Average (PAS Signal)
•
--
CO
Total
3
CL
400
200
—I—I—I—I—I—I—I—H
O)
O)
O)
O)
O)
O)
O)
O)
O)
O)
O)
O)
O)
O)
O)
O)
O)
O)
CN
CN
CN
CN
CN
CN
1
1
CN
CN
Day
Figure
26.
particles).
68
Long-term
1
1
1
1
1
1
1—H
1
1
1
oooooooooooooooo
oooooooooooooooo
S
CN
CN
O
N
O
O)
CO
-Î-
CN
o
co
o
-^
o
O)
i^
-^
o
-^
o
in
o
of Measurement
test of the PAS 2000
on a
constant aerosol
source
(carbon
6
Working
Area Measurements
and shows that the PAS offers
satisfying
reproducible results, especially
long period
over a
of
time.
Conclusions
6.5
It has been shown in two different field measurements that there is
between the
It is
measuring signal
possible
directly
a
a
PAS and the EC
concentration,
as
as a
conversion factor that allows to translate the online
The PAS
and
simple, fast,
yields
an
online
rapid changes
correlation
by coulometry.
signal
of the PAS
acquired,
the PAS
device for determination of the EC concentration in air.
cheap
signal
good
measured
into the actual EC concentration. Once this information has been
emerges
observe
obtain
to
of
a
with
a
time resolution of down to
of the ambient EC concentration. It
one
measures
therefore well suited for online surveillance of respirable ultrafine carbon
second, allowing
and is
continuously
particles
at
to
working
areas.
The
general properties
laboratory experiments
function of the
particle
sizes below 1 |im.
observed in field measurements have
under well controlled conditions. The
number concentration could be shown
Additionally,
the
reproducibility
and
also been
linearity
clearly
analyzed
of the PAS
signal
and for different
long-term stability
in
as a
particle
of the PAS could be
demonstrated.
It has to be
signal
on
pointed
out
that, while there is generally
and the EC concentration from
the type and
sensitivity
origin
of the
particles
of the aerosol that is
photoelectric charging
composition. However,
as
long
as
change significantly,
the PAS is
aerosol
is unknown
composition
or
correlation between the PAS
good
air, the respective conversion factor depends
This is related to
being analyzed.
method with
the chemical
qualified
in
a
regard
composition
for reliable
to
the
changes fundamentally,
certain
respective particle
of the measured
monitoring
a
particles
cross-
surface
does not
purposes of ambient air. If the
the
consistency
PAS data should be cross-checked with results from other sources, e.g.,
of the
acquired
coulometry.
69
7
Conclusions and Outlook
Conclusions and Outlook
7
It has been stressed that since the effects of very small airborne
the
particle SA,
of
judgement
particle
emissions based
be
can
sensitive to the
photoelectric charging
provide
much
airborne
on
example
such
(active) SA,
more
with
an
can
of
is
devices have
be obtained
by
presented
do.
measurements,
PAS
a
or
and
a
are
particle counting,
are
able to
as
for
DC, however, size-resolved
well trained
requires
in this work it
charging,
that
as
Very detailed information
size-resolved
quite expensive, bulky,
From the measurements
diffusion
or
PMX samples
SMPS system. In contrast to
measuring equipment usually
personnel.
course
mass
correlate with the
quite misleading. Measuring principles
information than
meaningful
particles
as
total
on
required by present-day legislation,
particles
can
be
seen
operating
that PAS and DC
great potential in assisting the evaluation of particle properties for both
a
emission measurements and
monitoring
of
working
area
air
quality, especially
with respect to
combustion aerosols.
The emission measurements
fuels have shown that the
on
selected modern combustion systems
principal part
of emitted
particles, weighted
concentrated in the nucleation and accumulation mode
be very small,
typical particle samples
can
nevertheless be present
(e.g.,
but
numerous
Especially
10
particles provide
with
regard
to
10
-
a
with J~30nm
becomes visible
particles
is formed
for
1/cm
for the
case
nm).
on a
number basis, is
While the total
number of small
of residential oil
can
with fossil
mass
particles
burners).
interact with its
of
may
Small
surrounding.
health effects, this fact should not be underestimated.
of soot
only
300
considerably high
considerable SA that
While the addition of small additive
improving burnout
a
(d<
operated
a
quantities
with d
directly
~
to
100 nm,
the fuel of EL oil burners is
a new
and
numerous
species
capable
of
of particles
from the additive material. The effect of the additive
mistuned burner,
emitting unnecessarily high
amounts
of soot. For
71
well maintained burners with little soot emissions, however, the creation of additive
dominant, and the employment of additives is
reduction of
emissions without side effects
particle
oil. It is remarkable that the
flame burner reduces
Investigation
particle
number emissions
modern GDI
a
designated
for
order of
operated
fuel-savings
It
that the GDI
seems
more
with
between state-of-the-art
gasoline
hence reduction of
emissions achieved
C02
and diesel
a
on a
conventional
emissions.
to
It
mode,
is
particles
engine
lies somewhere in
opposed by
are
S
GDI
a
be concluded that fuel
engine
GDI
yellow
of external air-fuel mixture
case
particle emissions,
can
the
In
the amount of emitted
than in the
engines.
by
by using highly purified
strategy for the sake of fuel-
DI
a
particle
to
regard
promising
more
of the H mode. Moreover,
case
is
orders of magnitude.
requirements,
particles
engine,
two
regard
than in the
magnitude higher
by
has shown that
engine
under low power
in the H mode also emits
preparation.
be achieved
can
of ECO oil instead of standard oil
use
has undesired consequences with
savings
one
of
recommendable. A much
not
particles
a
and
savings
notable increase
of particle emissions.
The
signal
PAS
for
coulometry,
has been
both
measurements at
compared
emission
of the air
applications
constant
is
of
of
working
measuring
of the PAS
determined
by coulometry.
measurements
the
values
comparison
insights
mass
on
the
concentrations,
time resolution and
area
the
air
analysis
quality,
findings
specific
a
sensor
are
signal
(if not misleading)
as
information
as
a
determined
as
and
providing input signals
It has to be stressed
should be calibrated for
required.
The calibration
awareness
that air
fast
of
engines,
for the electronic
are
confirmed with
specific
of the
quality
a
wide range
aerosol
easily
sources
if
obtained from
respective aerosol,
as
based
on
assessments
required by present-day legislation, provide only
on
a
a
that, while the ratio of PAS
factor is
with the EC concentration
area
A wide range of
operating cycles
from field measurements
for
sensor
long-term stability.
by
Since EC is
occur.
suitable
working
combustion aerosol is constant within
from this work lead to the
of total mass,
particles
of transient
and
engine
GDI
the PAS emerges
graphite particles.
on
particle concentrations,
The
high
of ventilation systems. The
and EC concentration for
absolute
72
particles,
with
quality
laboratory measurements
signal
measurements
imaginable, including
monitoring
steering units
EC
locations where elevated levels of diesel
reliable tracer for combustion
assessment
to
insufficient
the abundant number of nucleation and accumulation mode
7
Conclusions and Outlook
particles generated by
provide
necessary to
seems
be
to
a
particles
systems
to
or
certainly
diesel
nearly
are
voluntarily brought
is
a
of filters pose
to
be
a
possibilities
matter
consumers
of
that surround
a
reduction of the thermal
us.
with
are
on
research and
efficiency
development,
it is
The total SA
even
particle
filters. In the
case
on
the market,
equipped
with
a
exists to eliminate ultrafine
to pass
environmentally friendly
particle
but solutions
can
heavy-duty
of passenger and
particle
emissions
smallest
of combustion
demonstrated in Switzerland, where
without maintenance for 80'000 km. These
political willingness
to use
particles
should be taken. The french automobile manufacturer
diesel vehicle
operational
the
filters eliminate the emissions of
challenges
examples
being equipped
same measures
on
particle effects,
for this purpose.
100 %. Drawbacks like
be found. Positive
vehicles, the
technical
measure
high-efficiency particle
clogging
engines
promised
additional information
qualified
It is known that
modern combustion systems. With respect to
freight
Peugeot has
filter system that is
examples
quickly
and
the necessary laws that force both
show that
sustainably.
producers
It
and
and safe combustion systems.
73
Appendix
Appendix
A.1
Published material
Selected
of this work have been considered for
chapters
information for retrieval of the
publication.
The necessary
is listed in table 7.
respective publications
Status
Chapter
as
of
September
Reference
Title
2002
Authors: K.
Ultrafine Particle Emissions
4
Z.
Qian,
of Residential Oil Burners:
Journal: Combustion Science and
Influence of Burner
Fuel, and Additives
Technology (CST)
Issue: Vol. 174 (2002) No. 9, p. 49-66
Publisher: Taylor & Francis Group
SI Direct
Chapter 8 in: Particulates of Piston
Engine Combustion Processes.
Final Report 2001. KTI Project
Type,
Injection Engine
Particulate Analysis
5
Przybilla,
U. Matter, H. Burtscher
4207.2
in
print
published
KTS, 1999-2001
Przybilla, W. Berkhahn,
Burtscher, D. Dahmann,
Authors: K.
H.
6
Monitoring diesel
particulates in working
areas with the photoelectric
Journal: Gefahrstoffe /
aerosol
Issue: 62
sensor
U. Matter, P. Rietschel
Reinhaltung
(Air Quality Control)
(2002) Nr. 6 Juni,
published
der Luft
-
p. 279-284
Publisher:
Table 7. Information
A.2
on
Springer
VDI
Verlag
published material.
Particle diameters
Airborne
particles,
irregular shapes.
advanced and
and is useful
and
especially particle agglomerates,
A discrimination based
costly microscopic imaging
mainly
on
the basis of random
on
is
shape
methods
can
have very
possible only
(e.g.,
to
complicated
some
transmission electron
extent
and
with
microscopy)
sampling.
75
Appendix
Online discrimination of airborne
according
equivalent
to an
object (e.g.,
a
question.
The
property
and
sphere)
yield
table
differently
aerosol
particles
particles corresponding
magnitude.
8.
Two
In
frequently
this
used
electrical
mobility
(equivalent)
Table 8.
These
specific equivalent
differently
equivalent
defined
diameters
by
means
equivalent
a
spherical particle
diameter of
singly charged
spherical particle that has the
are
usually
not
diameter of the
to
the
are
electrical
same
listed in
mobility
(section 3.1.3).
Property
depends on
particle mass and
Application
cascade
impactor
density
a
mobility in an
electric field as the respective
singly charged particle
same
electrical
independent of
mass
and
in
specific physical
physical properties
of the SMPS system
a
a
particle
diameter need not be identical to
diameters and their
density of 1 g/cm3 that
has the same settling velocity
as the respective particle
with
density
DMA, integral
part of the SMPS
Example of equivalent diameters for the characterization of small airborne particles
with respect to "size".
76
one
diameters.
linked to
particles
(idealized)
an
the actual aerosol
as
necessarily
Definition
diameter of
diameter
a
determined
as
Diameter
aerodynamic
(equivalent)
to
defined
of
diameter is the diameter of
physical properties
are
the classification of
on
work, all measured particle diameters refer
(equivalent) diameter,
diameter
same
equivalent
respective measuring principles
interchangeable:
those
diameter. An
that has the
is based
particles
Appendix
A.3
Measuring
Table
9
coulometric
current
contains
analyses
devices
information
were
kindly
disk dilution
unit
devices.
measuring
EMPA
,
SUVA
,
Gravimetric
and BGN
and
according
to
Specification
MD 19-1Eand
MD
Photoelectric aerosol
(PAS)
Diffusion
sensor
charging
(DC)
SMPS: DMA
SMPS: CPC
Table 9.
19-2Eby
Engineering AG
Prototype of
as
sensor
Details
10 cavities disk
Matter
Thermodesorber
PAS 2000
[11]
by EcoChem
operated
at 330 °C
water cooled
Range:
5000 fA
LQ1-DC by
Matter
Engineering AG
-
S/N 100'221
3071
High flow:
byTSI
3025A
15
Low flow: 3
S/N 1092
1.5 l/min.
vs.
vs.
Up-/Downscan:
0.3 l/min.
60
sec.
/ 30
sec.
by TSI
-
S/N 253
Employed measuring
Schweizerische
ETH Zürich
described in
S/N 137
Eidgenossische Matenalprufungs-
***
by
used
standards.
Rotating
**
the
carried out
Item
*
about
devices.
und
Forschungsanstalt,
Unfallversicherungsanstalt,
Berufsgenossenschaft Nahrungsmittel
CH-8600 Dubendorf /
CH-6005 Luzern /
Gravimetry, chapter
Coulometry, chapter
und Gaststatten, D-68165 Mannheim /
5
5
Chapter
6
77
Appendix
A.4
Fuel and additive
composition
Table 10 contains information about the used fuel and additive. The examined EL oil types
are
primarily
used in
also in Scandinavia,
Europe, especially
Germany, France, Austria,
Belgium, Luxembourg, Greece, Poland,
type of oil is also known
Heating
in
as
and the Czech
Industrial Fuel Oil,
Light Heating Oil, Light
and Switzerland, but
Republic.
Light Gasoil,
or
This
Home
Oil.
Item
Value
Description
mg/kg
water content
130
total contamination
3
sulfur content
0.091 mass-%
nitrogen
121
mg/kg
Standard EL oil
content
mg/kg
mg/kg
water content
85
total contamination
2
sulfur content
0.017 mass-%
nitrogen
57
mg/kg
ECO EL oil
Table 10. Oil and additive
color of the
respective
thermal radiation of
78
chapter
4
combustion flame. The
glowing
flame burners achieve better
soot
composition.
Classification of oil burners
The classification of oil burners in
injected
mg/kg
Fe(C5H5)2
ferrocene
Additive
A.5
content
soot
(EC) particles.
mixing
(yellow
yellow
In
of air and fuel
are
emitted.
blue flame
coloration of
comparison
to
by vaporization
into the combustion chamber. This leads to
particles
vs.
a
a
burners)
refers to the
flame is attributed to
yellow
flame burners, blue
of the fuel
droplets
cleaner combustion in the
sense
that
are
that less
Appendix
Burner Y-R in
are
designed
4 is
chapter
a
flame burner,
yellow
for reduction of NOx emissions
additionally equipped
by recirculating
main combustion chamber. This process reduces the
a
portion
caused
by high
flame temperatures
The motion of small
particles (diameter
conditions and low velocities (v
•
d/2
•
Force
«
of
speed
d
<
F
oc
d
Validity: 1
on
particle due
to the gas
•
it:
2
,
proportional
nm <
d
<
40
to surface
:
viscosity
velocity
at
the surface of small
resistance force of the gas
is valid for the transition
«
X and d/2
»
acting
the formation of
gas
»
free
(mean
two
path X )
at
standard
regimes [37]:
X : Cunningham regime
acting on particle
surrounding it:
Force
due to the gas
6nr\(d/2)v
d, proportional
oc
(2)
to diameter
on
the
of gas
of particle in gas
mean
is the formula of Stokes (F
occurs
retarding
Validity: 100nm<J< 1.6 |im
nm
free
A, Q: constants, depending
gas molecules
d/2
i.e., F
area
X:
(2)
a
F
v:
Formula
in
6%V[(d/2)2v
(A + Q)X
_
of the flue gas into the
area
sound) is divided into
•
r\
d/2
|im)
1
X : free molecular regime
acting
surrounding
i.e., F
«
FGR. FGR
(thermal NOx).
Calculation of the active surface
A.6
a
combustion temperature and lowers
peak
the percentage of oxygen in the combustion air-fuel mixture, thus
NOx
with
=
on
path
the
scattering
-6nr\(d/2)v),
particles,
is
moving particle.
region d/2~'k
and
process
corrected for
proportional
The
approximates
to
"slip". Slipping
-j—,
and reduces the
following empirical
formulae
(1)
and
of
(2)
formula
for the
(3)
cases
X, respectively:
79
Appendix
6m\(d/2)v
_
^
d/2
We define S
=
%(d/2)2
in Formula
6r|v
s
(1)
as
for S
yields
d/2
as a
K(A
=
,
a
+
l+A
X
172
_l
+
+
FV
d/2
X
particle
Q)X(d/2)
X
r,
ô
^
function of the
172
The parameters for air at standard conditions
are
( b d/2\
expl-^^J
[1]: X
A
Q
b
80
(1)
=
(3):
6m\(d/2)v
the active SA
s
X
the active SA and equate
=
V
Solving (4)
rV
d/2
=
=
66
nm
1.17
=
0.525
=
0.78
y
diameter d:
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Acknowledgements
Acknowledgements
I thank Hans
Christoph Siegmann
his aerosol group,
even
would break up
before
administrative
his
opportunity
for
me.
that he would retire and that the group
Since
I thank them for
thanks to Heinz Burtscher for
to
Ulrich Matter
participation
Ph. D. in
to carry out my
this
circumstance
so
doing. Furthermore,
investing
lot of time and
a
work, for many helpful discussions and lots of good advice.
willingness
different
anticipated
concluded my thesis.
I
responsibility
special
my written
it could be
though
the
me
created
some
I thank Danilo for
of the final examination.
taking charge
owe
giving
inconvenience, Danilo Pescia and Martin Landolt kindly accepted the
administrative
I
for
take
was
my
in several
projects
discussions and
the
on
position
supervisor, already
since my
interesting projects. Although
propositions,
and for
in
reviewing
I further thank him for
of the co-examiner.
time, he still managed
at a
patience
he
diploma thesis,
was
to squeeze in
reviewing
and
for my
arranged
involved in at least three
always
the necessary time for
my written reports. I
helpful
greatly acknowledge
his
support.
I further thank the members of the former aerosol group: Gerda
care
Rüegg-Schibler
of administration, Leo Scherrer for advice in electronics, Konstantin
answering
all
constructive
inventory
grateful
questions
problems.
and
getting
that he took
related to
chemistry,
and Pierre Cohn for his
Pierre furthermore had the
of this while I
was
of
unpleasant duty
rid of all the material that had accumulated
care
help
busy analyzing
over
data and
and Stefan Riesen
electrons). Special
(of
the other
Siegmann
thanks goes to Martin Fierz and
guide
in Oaxaca and
pleasant
hospitality
company
good
during
our
mechanical and
the group
the years. I
am
very
my thesis.
dealing
not
with
only
spin polarized
for their
company in the office and
in Sils and Montafon.
for
Fierz, Alejandro Keller,
Alejandro Keller,
with respect to work-related issues, but also for their
occasions: I thank Martin for his
group,
taking
Siegmann
dissolving
writing
I also want to thank my fellow Ph. D. students in the group, Martin
Georg Skillas,
on
for
Alejandro
scientific visit to
was a
on
help
other
great
Braunschweig,
tour
among
many other occasions.
I further thank Markus
had to share
Kasper and Thomas Mosimann of
measuring equipment
with Thomas,
a
lot of
Matter
equipment
Engineering
AG. Since I
had to be shifted to and
84
Acknowledgements
from ETH
Hönggerberg quite
and efficient, also when
With respect to
Jungbluth
financed
Chapter
6 is based
Rietschel. Further
on
not
acknowledgements
corresponding publication,
helpfulness
on
mention them
In the
both
by
beginning
designated
the
name
help
a
I thank my
several measurements in
the
colleagues
since I
of
Wolfgang Berkhahn,
appendix,
I have not mentioned
afraid of unintentionally
particles
in
experiments
the
field of
of Paul G Seiler, Gert Viertel,
lot of time in
optimizing
chapter
was
4
were
Dirk
Dahmann, and
Peter
chapter
6
are
mentioned
section A.l.
and work-related occasions.
am
project
help.
related to the measurements of
of my Ph. D., I conducted
Röser, who invested
Finally,
see
personal
for detection
acknowledge
85
I thank him for his
and Hubert
Hornig
for constructive contributions. The oil burner
contributions from
I thank all my friends and
and
together.
Germany. Furthermore,
by Zhiqiang Qian.
uncomplicated
was
would like to express my thanks to Michael
Germany,
Octel GmbH,
by
did measurements
chapter 4,1
of Octel GmbH,
carried out
in the
we
often. Nevertheless, team work with Thomas
with
high
Hanspeter
so
far for their
They
may
leaving
good
forgive
someone
company
me
that I do
out.
microstrip detectors, originally
energy
von
physics.
I
gratefully
Gunten, and especially Ulf
detection electronics for my purposes.
parents and my sister for their unconditional support.
Curriculum Vitae
Curriculum Vitae
Name:
Karl Richard
Nationality:
Germany
1979
1983
1984
-
-
-
Przybilla
17 in
Manhasset,
York, USA.
1973
Born
1983
Elementary
school in Schaanwald, Liechtenstein.
1984
Elementary
school in Mauren, Liechtenstein.
1992
Liechtensteinisches
January
New
Gymnasium (secondary
school)
in
Vaduz,
Liechtenstein.
1992
-
(school leaving examination,
classical with
1992
Matura
1998
Student of
experimental physics at the Swiss
Technology (ETH) in Zürich, Switzerland.
1998
Diploma
Diploma
Typus
in
B
Latin).
Federal Institute of
experimental physics (Dipl. Phys. ETH).
thesis: "Einfluss
von
Treibstoffzusätzen auf den Verbren¬
nungsvorgang in
Prof. Dr. H. C.
Leichtöl-Feuerungen", conducted in the group of
Siegmann at the Laboratory of Solid State Physics,
ETH
1998
-
2002
Zürich, Switzerland.
Ph. D. student and
Physics,
Siegmann.
ETH
teaching
assistant at the
Zürich, Switzerland, in the
Laboratory
of Solid State
group of Prof. Dr. H. C.
Zürich, April 2002
86