AE-213
UDC 543.53:546.49
CO
CN
•
Low Temperature Irradiation Applied to
Neutron Activation Analysis of
Mercury In Human Whole Blood
D. Brune
This report is intended for publication in a periodical. References
may not be published prior to such publication without the
consent of the author.
AKTIEBOLAGET ATOMENERGI
STOCKHOLM, SWEDEN 1966
AE-213
LOW TEMPERATURE IRRADIATION APPLIED TO NEUTRON
ACTIVATION ANALYSIS OF MERCURY IN HUMAN WHOLE BLOOD
Dag Brune
AB Atomenergi, Studs vik, Sweden
Summary
The distribution of mercury in human whole blood has been studied
by means of neutron activation analysis.
During the irradiation procedure the samples were kept at low
temperature by freezing them in a cooling device in order to prevent
interferences caused by volatilization and contamination.
The mercury activity was separated by means of distillation and
ion exchange techniques.
Printed and distributed in February 1966.
LIST OF CONTENTS
Page
Introduction
3
Experimental
4
Results and discussions
4
Acknowledgements
5
Appendix
5
Table 1
6
References
7
- 3 -
Introduction
The determination of mercury in small quantities has in recent
times attracted increasing attention. Mention may here be made of,
for example, cases of poisoning in connection with seed treatment with
fungicides [1].
Several methods for the determination of mercury in biological
material by means of neutron activation analysis are now available
F2-6], In this connection separation techniques based on distillation,
extraction, exchange reactions, precipitation and electrolytic deposition are employed which may permit an accurate determination of mercury,
However, the analysis is still encumbered with certain problems
attributed to the volatility of various mercury compounds. Thus, considerable losses of mercury during the drying of organic matter have
been reported [3, 7, 8], The irradiation of wet biological samples is
otherwise connected with certain disadvantages. The pressure built up
by radiolysis in the sealed ampoules may give rise to losses of volatile
compounds when the ampoules are opened if the pressure is not decreased by cooling, in for example, liquid nitrogen before opening.
Losses of mercury due to volatilization from aqueous solutions
(e.g. biological fluids or water), may be even more pronounced. This
would occur, for example, during an evaporization performed in order
to concentrate the sample before activation and also during the subsequent irradiation step. Thus, from solutions containing chloride or
sulphate ions in concentrations of 100 p. p. m. , volatilization losses of
more than 50 per cent have been observed by the author when heating
such solutions at temperatures of about 60
C for 12 h. This tempera-
ture is almost the same as that which arises in aqueous samples in irradiation positions generally applied for such samples in the reactor Rl,
Stockholm.
During the irradiation procedure, reactive species are formed
in water producing, for example, hydrogen peroxide which may, moreover, contribute to the volatilization processes, though probably not to
any appreciable extent.
However, if the activation is performed at a low temperature by
freezing the samples in a cooling device during neutron irradiation,
these losses, as well as the contamination of the samples from the con-
- 4-
tainer walls, can be avoided [9]. In this way the accuracy of the analysis may be improved.
Low temperature irradiation has been applied in the present investigation to the determination of the mercury content of human whole
blood.
Using this technique the mercury may be determined with .a
standard deviation of a single value of 7 per cent [ 9 j .
Experimental
Blood samples of about 2 ml were collected in polyethylene containers from 20 healthy blood donors. The samples were irradiated
1Z
2
in a thermal neutron flux of about 2 x 1 0
for 1 3 h at a temperature of about - 40
n/cm
sec in Rl, Stockholm
C in a cooling device described
elsewhere F9]. After the "cold" irradiation procedure, the samples
were allowed to melt for a short time in order to remove a thin surface layer which may have been contaminated by the container surface. The samples were then transferred to a closed system and destroyed with H ? SO. and H ? O ? . The mercury activity was then separated
by means of distillation and ion exchange techniques before gammaspectrometric measurements being undertaken [5]. The analysis was
assayed by means of the nuclide Hg
The mercury standard consisted of an aqueous solution of HgSO .
with a volume of 2 ml (~ equal to the volume of the blood samples) which
was also irradiated in the frozen state.
Results and discussion
The amounts of mercury in the 20 samples of human whole blood
investigated are given in table 1. These values are nearly consistent
with a skew distribution and the median, amounting to 0. 011 |j,g/g, has
consequently been chosen to represent the central value. The range of
the mercury concentrations, expressed as the ratio of the highest and
lowest values, corresponded to a factor of 8.
The concentration of various elements in trace quantities in mammalian tissues, moreover, often exhibits a skew distribution [8,10].
The mercury content of human heart material also showed such a distribution, with about the same range as that obtained in the present
investigation [8].
Yield: 96 per cent
- 5 -
The median value obtained for the mercury content in whole
blood is about twice the mean value previously reported by Comar et al.
who also used neutron activation analysis in the investigation [4].
At concentrations down to 0. 05 p. p. m. , mercury can also be determined using non-radioactivation methods [7].
Stock, who also examined the mercury content of human whole
blood, applied a method based on microscopic observations [11]. In
his investigation, a mean value was obtained which was nearly equal to
the median value of the present investigation.
In Stock' s work, the influence of the amalgam content of teeth on
the mercury concentration of the blood was also studied. The presence
of amalgam did not, however, seem to affect this concentration. On the
other hand, the mercury content in various organs was appreciably increased in the case of persons with amalgam fillings.
Acknowledgements
The author is greatly indebted to Mrs. B. Bivered for skilful
technical assistance and to Miss B. Ullman at the blood bank at
Nyköpings Lasarett for providing the samples.
Appendix
In the determination of mercury in water, the freezing technique
was found to be suitable in combination with the separation technique
involving exchange reactions described by Kim and Silverman [2].
However, this separation technique was slightly modified by increasing
the exchange time two-fold (10 min.) and the mercury content fourfold (0. 2 ml), resulting in a recovery of 98 per cent with a standard
deviation of a single value of 1 per cent.
- 6 -
Table 1
Sample Age
(y)
Sex
Mercurycontent
(n-g/g)
S ampla / g e
(y)
Sex
Mercurycontent
(ve/e)
1
41
?
0.003
11
39
2
43
tf
0. 003
12
34
3
21
<f
0. 004
13
35
d1
0. 013
4
31
?
0. 006
14
35
?
0. 014
5
41
<?
0.. 008
15
37
6
37
<?
0. 008
16
37
<$
0. 017
7
31
<t
0. 010
17
40
<?
0. 018
8
30
cf
0. 010
18
29
<?
0. 020
9
31
d1
0. 010
19
37
<f
0. 023
10
29
0. Oil
20
49
<?
0. 024
d"
0. Oil
0.011
0. 015
Mercury content of human whole blood, expressed in jj,g mercury
per g whole blood. Median value: 0. 011 |ig/g, Range: 8.
- 7 -
References
1.
ULFVARSON, U,
Kvicksilver, aldrin och dieldrin i fasaner.
Sv. Kem. Tids. 77 (1965) 235.
2.
KIM, C K and SILVERMAN, J,
Determination of Mercury in wheat and tobacco leaf by neutron
activation analysis . . .
Anal. Chem. 3^(1965) 1616.
3.
WESTERMARK, T and SJÖSTRAND, B,
Activation analysis of Mercury.
Int. J. Appl. Rad. Isotop. £(1960) 1.
4.
COMAR, D, LE POEC, C, JOLY, M and KELLERSHOHN, C,
L1 analyse par radioactivation . . .
Bull. Soc. Chim. France (1962) 56.
5.
WESTER, P O , BRUNE, D and SAMSAHL, K,
Radiochemical recovery studies of a separation scheme for 2 3
elements in biological material.
Int. J. Appl. Rad. Isotop.]_5_ (l 964) 59.
6.
SJÖSTRAND, B,
Simultaneous determination of Mercury and Arsenic in biological
and organic materials by activation analysis.
Anal. Chem. Vol. 36 (1964) 814.
7.
JOHNSON, WC, GAGE, J C et al. ,
Determination of small amounts of Mercury in organic matter.
Analyst 90 (1965) 515.
8.
WESTER, P O,
Concentration of 24 trace elements in human heart tissue determined by neutron activation analysis.
Scand. J. Lab. Clin. Invest. JJ\(l 965) 357.
9.
BRUNE, D and LANDSTRÖM, O,
Radiochim. Acta. (in P r e s s . )
10.
TIPTON, I H and COOK, M J,
Trace elements in human tissue P . 2.
Health Phys. ±{\9G3) 103.
11 .
STOCK, A,
Mercury content of the human body.
Biochem. Z. !3£4 (l 940) 73.
LIST OF PUBLISHED AE-REPORTS
1—135. (See the back cover earlier reports.)
136. Ejection of uranium atoms from UO2 by fission fragments. By G. Nilsson.
1964. 38 p. Sw. cr. 8:—.
137. Personell neutron monitoring at AB Atomenergi. By S. Hagsgård and
C.-O. W i d e l l . 1964. 11 p. Sw. cr. 8:—.
138. Radiation induced precipitation in iron. By B. Solly. 1964. 8 p. Sw. cr.
8:—.
139. Angular distributions of neutrons from (p, nl-reactions in some mirror
nuclei. By L. G . Strömberg, T. Wiedling and B. Holmqvist. 1964. 28 p.
Sw. cr. 8:—.
140. An extended Greuling-Goertzel approximation with a Pn -approximation
in the angular dependence. By R. Håkansson. 1964. 21 p. Sw. cr. 8:—.
141. Heat transfer and pressure drop with rough surfaces, a literature survey.
By A . Bhattachayya. 1964. 78 p. Sw. cr. 8:—.
142. Radiolysis of aqueous benzene solutions. By H. Christensen. 1964. 50 p.
Sw. cr. 8.—.
143. Cross section measurements for some elements suited as thermal spectrum indicators: Cd, Sm, Gd and Lu. By E. Sokolowski, H. Pekarek and
E. Jonsson 1964. 27 p. Sw. cr. 8:—.
144. A direction sensitive fast neutron monitor. By B. Antolkovic, B. Holmqvist and T. Wiedling. 1964. 14 p. Sw. cr. 8:-—.
145. A user's manual for the NRN shield design method. By L. Hjärne. 1964.
107 p. Sw. cr. 10:—.
146. Concentration of 24 trace elements in human heart tissue determined
by neutron activation analysis. By P. O. Wester. 1964. 33 p. Sw. cr. 8:—.
147. Report on the personnel Dosimetry at AB Atomenergi during 1963. By
K.-A. Edvardsson and S. Hagsgård. 1964. 16 p. Sw. cr. 8:—.
148. A calculation of the angular moments of the kernel for a monatomic gas
scatterer. By R. Håkansson. 1964. 16 p. Sw. cr. 8 —.
149. An anion-exchange method for the separation of P-32 activity in neutron-irradited biological material. By K. Samsahl. 1964. 10 p. Sw. cr
6s
150. Inelastic neutron scattering cross sections of Cu'" and Cu in the energy
region 0.7 to 1.4 MeV. By B. Holmqvist and T. Wiedling. 1964. 30 p.
Sw. cr. 8:—.
151. Determination of magnesium in needle biopsy samples of muscle tissue
by means of neutron activation analysis. By D. Brune and H. E. Sjöberg.
1964. 8 p. Sw. cr. 8:—.
152. Absolute El transition probabilities in the dofermed nuclei Yb 1 " and
HP». By Sven G. Malmskog. 1964. 21 p. Sw. cr. 8:—.
153. Measurements of burnout conditions for flow of boiling water in vertical
3-rod and 7-rod clusters. By K. M. Becker, G. Hernborg and J. E. Flinta.
1964. 54 p. Sw. cr. 8 1 154. Integral parameters of the thermal neutron scattering law. By S. N.
Purohit. 1964. 48 p. Sw. cr. 8:—.
155. Tests of neutron spectrum calculations with the help of foil measurmenfs
in a D2O and in an H2O-moderated reactor and in reactor shields of
concrete and iron. By R. Nilsson and E. Aalto. 1964. 23 p. Sw. cr. 8:—.
156. Hydrodynamic instability and dynamic burnout in natural circulation
two-phase flow. An experimental and theoretical study. By K. M. Becker. S. Jahnberg, I. Haga, P. T. Hansson and R. P. Mathisen. 1964. 41 p.
Sw. cr. 8:—.
157. Measurements of neutron and gamma attenuation in massive laminated
shields of concrete and a study of the accuracy of some methods of
calculation. By E. Aalto and R. Nilsson. 1964. 110 p. Sw. cr. 10:—.
the Be' (p,n) B'
158. A study of the angular distributions of neutrons from
reaction at low proton energies. By. B. Antolkovic 1 , B. Holmqvist and
T. Wiedling. 1964. 19 p. Sw. cr. 8 : - .
159. A simple apparatus for fast ion exchange separations. By K. Samsahl.
1964. 15 p. Sw. cr. 8 : M
H
160. Measurements of the Fe (n, p) M n
reaction cross section in the neutron
energy range 2.3—3.8 MeV. By A. Lauber and S. Malmskog. 1964. 13 p.
Sw. cr. 8:—.
161. Comparisons of measured and calculated neutron fluxes in laminated
iron and heavy water. By. E. Aalto. 1964. 15 p. Sw. cr. 8:—.
162. A needle-type p-i-n junction semiconductor detector for in-vivo measurement of beta tracer activity. By A. Lauber and B. Rosencrantz. 1964. 12 p.
Sw. cr. 8:—.
163. Flame spectro photometric determination of strontium in water and
biological material. By G. Jönsson. 1964. 12 p. Sw. cr. 8:—.
164. The solution of a velocity-dependent slowing-down problem using case's
eigenfunction expansion. By A. Claesson. 1964. 16 p. Sw. cr. 8:—.
165. Measurements of the effects of spacers on the burnout conditions for
flow of boiling water in a vertical annulus and a vertical 7-rod cluster.
By K. M. Becker and G. Hemberg. 1964. 15 p. Sw. cr. 8:—.
166. The transmission of thermal and fast neutrons in air filled annular ducts
through slabs of iron and heavy water. By J. Nilsson and R. Sandlin.
1964. 33 p. Sw. cr. 8:—.
167. The radio-thermoluminescense of CaSOi: Sm and its use in dosimetry.
By B. Bjämgard. 1964. 31 p. Sw. cr. 8:—
168. A fast radiochemical method for the determination of some essential
trace elements in biology and medicine. By K. Samsahl. 1964. 12 p. Sw.
cr. 8:—.
169. Concentration of 17 elements in subcellular fractions of beef heart tissue
determined by neutron activation analysis. By P. O . Wester. 1964. 29 p.
Sw. cr. 8:—.
170. Formation of nitrogen-13, fluorine-17, and fluorine-18 in reactor-irradiated
H2O and D2O ana applications to activation analysis and fast neutron
flux monitoring. By L. Hammar and S. Forsen. 1964. 25 p. Sw. cr. 8:—.
171. Measurements on background and fall-out radioactivity in samples from
the Baltic bay of Tvären, 1957—1963. By P. O. Agnedal. 1965. 48 p. Sw.
cr. 8:—
172. Recoil reactions in neutron-activation analysis. By D. Brune. 1965. 24 p.
Sw. cr. 8:—
173. A parametric study of a constant-Mach-number MHD generator with
nuclear ionization. By J. Braun. 1965. 23 p. Sw. cr. 8:—.
174. Improvements in applied gamma-ray spectrometry with germanium semiconductor dector. By D. Brune, J. Dubois and S. Hellström. 1965. 17 p.
Sw. cr. 8:—.
175. Analysis of linear MHD power generators. By E. A. Witalis.,1965. 37 p.
Sw. cr. 8:—.
176. Effect of buoyancy on forced convection heat transfer in vertical channels — a literature survey. By A. Bhattacharyya. 1965. 27 p. Sw. cr. 8:—.
177. Burnout data for flow of boiling water in vertical round ducts, annuli
and rod clusters. By K. M. Becker, G. Hernborg, M. Bode and O . Erikson. 1965. 109 p. Sw. cr. 8:—.
178. An analytical and experimental study of burnout conditions in vertical
round ducts. By K. M. Becker. 1965. 161 p. Sw. cr. 8:—.
179. Hindered El transitions in Eu1K and Tb151. By S. G. Malmskog. 1965. 19 p.
Sw. cr. 8:—.
180. Photomultiplier tubes for low level Cerenkov detectors. By O. Strindehag. 1965. 25 p. Sw. cr. 8:—.
181. Studies of the fission integrals of U235 and Pu239 with cadmium and
boron filters. By E. Hellstrand. 1965. 32 p. Sw. cr. 8:—.
182. The handling of liquid waste at the research station of Studsvik, Sweden.
By S. Lindhe and P. Linder. 1965. 18 p. Sw. cr. 8:—.
183. Mechanical and instrumental experiences from the erection, commissioning and operation of a small pilot plant for development work on
aqueous reprocessing of nuclear fuels. By K. Jönsson. 1965. 21 p. Sw.
cr. 8:—.
184. Energy dependent removal cross-sections in fast neutron shielding
theory. By H. Grönroos. 1965. 75 p. Sw. cr. 8:—.
185. A new method for predicting the penetration and slowing-down of
neutrons in reactor shields. By L. Hjärne and M. Leimdörfer. 1965. 21 p.
Sw. cr. 8:—.
186. An electron microscope study of the thermal neutron induced loss in
high temperature tensile ductility of Nb stabilized austenitic steels.
By R. B. Roy. 1965. 15 p. Sw. cr. 8:—.
187. The non-destructive determination of burn-up means of the Pr-144 2.18
MeV ga.nma activity. By R. S. Forsyth and W. H. Blackadder. 1965.
22 p. Sw. cr. 8:—.
188. Trace elements in human myocardial infarction determined by neutron
activation analysis By P. O. Wester. 1965. 34 p. Sw. cr. 8:—.
189. An electromagnet for precession of the polarization of fast-neutrons.
By O. Aspelund, J. Björkman and G. Trumpy. 1965. 28 p. Sw. cr. 8:—.
190. On the use of importance sampling in particle transport problems. By
B. Eriksson. 1965. 27 p. Sw. cr. 8:—.
191. Trace elements in the conductive tissue of beef heart determined by
neutron activation analysis. By P. O. Wester. 1965. 19 p. Sw. cr. 8:—.
192. Radiolysis of aqueous benzene solutions in the presence of inorganic
oxides. By H. Christensen. 12 p. 1965. Sw. cr. 8:—.
193. Radiolysis of aqueous benzene solutions at higher temperatures. By
H. Christensen. 1965. 14 p. Sw. cr. 8:—.
194. Theoretical work for the fast zero-power reactor FR-0. By H. Häqqblom.
1965. 46 p. Sw. cr. 8:—.
195. Experimental studies on assemblies 1 and 2 of the fast reactor FRO.
Part 1. By T. L. Andersson, E. Hellstrand, S-O. Londen and L. 1. Tirén.
1965. 45 p. Sw. cr. 8:—.
196. Measured and predicted variations in fast neutron spectrum when penetrating laminated Fe-D ; O. By E. Aalto, R. Sandlin and R. Fräki. 1965.
20 p. Sw. cr. 8:—.
197. Measured and predicted variations in fast neutron spectrum in massive
shields of water and concrete. By E. Aalto, R. Fräki and R. Sandlin. 1965.
27 p. Sw. cr. 8:—.
198. Measured and predicted neutron fluxes in, and leakage through, a configuration of perforated Fe plates in D2O. By E. Aalto. 1965. 23 p. Sw.
cr. 8:—.
199. Mixed convection heat transfer on the outside of a vertical cylinder.
By A. Bhattacharyya. 1965. 42 p. Sw. cr. 8:—.
200. An experimental study of natural circulation in a loop with parallel
flow test sections. By R. P. Mathisen and O. Eklind. 1965. 47 p. Sw.
cr. 8:—.
201. Heat transfer analogies. By A. Bhattacharyya. 1965. 55 p. Sw. cr. 8:—.
202. A study of the "384" KeV complex gamma emission from plutonium-239.
By R. 5. Forsyth and N. Ronqvist. 1965. 14 p. Sw. cr. 8:—.
203. A scintillometer assembly for geological survey. By E. Dissing and O.
Landström. 1965. 16 p. Sw. cr. 8:—.
204. Neutron-activation analysis of natural water applied to hydrogeology.
By O. Lundström and C. G . Wenner. 1965. 28 p. Sw. cr. 8:—.
205. Systematics of absolute gamma ray transition probabilities in deformed
odd-A nuclei. By S. G . Malmskog. 1965. 60 p. Sw. cr. 8:—.
206. Radiation induced removal of stacking faults in quenched aluminium.
By U. Bergenlid. 1965. 11 p. Sw. cr. 8:—.
207. Experimental studies on assemblies 1 and 2 of the fast reactor FRO.
Part 2. By E. Hellstrand, T. L. Andersson, B. Brunfelter, J. Kockum, S-O.
Londen and L. I. Tirén. 1965. 50 p. Sw. cr. 8:—.
208. Measurement of the neutron slowing-down time distribution at 1.46 eV
and its space dependence in water. By E. Möller. 1965. 29. p.Sw.cr.8:—.
209. Incompressible steady flow with tensor conductivity leaving a transverse
magnetic field. By E. A. Witalis. 1965. 17 p. Sw. cr. 8:—.
210. Methods for the determination of currents and fields in steady twodimensional MHD flow with tensor conductivity. By E. A. Witalis. 1965.
13 p. Sw. cr. 8 : - .
211. Report on the personnel dosimetry at AB Atomenergi during 1964. By
K. A. Edvardsson. 1966. 15 p. Sw. cr. 8:—.
212. Central reactivity measurements on assemblies 1 and 3 of the fast
reactor FRO. By S-O. Londen. 1966. 58 p. Sw. cr. 8:—.
213. Low temperature irradiation applied to neutron activation analysis of
mercury in human whole blood. By D. Brune. 1966. 7 p. Sw. cr. 8:—.
Förteckning över publicerade AES-rapporter
1. Analys medelst gamma-spektrometri. Av D. Brune. 1961. 10 s. Kr 6:—.
2. Bestrålningsförändringar och neutronaimosfär i reaktortrycktankar —
några synpunkter. Av M. Grounes. 1962. 33 s. Kr 6:—.
3. Studium av sträckgränsen i mjukt stål. Av G. Oslberg och R. Attermo.
1963. 17 s. Kr 6 : - .
4. Teknisk upphandling inom reaktorområdet. Av Erik Jonson. 1963. 64 s.
Kr 8:~~.
5. Ågesta Kraftvärmeverk. Sammanställning av tekniska data, beskrivningar
m. m. för reaktordelen. Av B. Lilliehöök. 1964. 336 s. Kr 15:—.
Additional copies available al the library of AB Atomenergi, Studsvik,
Nyköping, Sweden. Transparent microcards of the reports are obtainable
through the International Documentation Center, Tumba, Sweden.
EOS-tryckerierna, Stockholm 1966