Electronic Supplementary Material (ESI) for Physical Chemistry Chemical Physics.
This journal is © the Owner Societies 2014
Electronic supplementary information:
Catalytic oxidation of CO with N2O on isolated copper cluster anions
Shinichi Hirabayashi,a Masahiko Ichihashi*b
a
East Tokyo Laboratory, Genesis Research Institute, Inc., 717-86 Futamata, Ichikawa,
Chiba 272-0001, Japan
b
Cluster Research Laboratory, Toyota Technological Institute: in East Tokyo
Laboratory, Genesis Research Institute, Inc., 717-86 Futamata, Ichikawa, Chiba
272-0001, Japan. E-mail: [email protected]
1
Figure S1: Mass spectra obtained in the reactions of Cu9− with N2O under a multiple
collision condition (N2O pressure of 1×10−3 Torr) [panel (a)] and with a mixture of
N2O (1×10−3 Torr) and CO (5×10−3 Torr) [panel (b)]. The intensities are normalized to
the total ion intensity. Panel (c) shows a difference spectrum obtained by subtracting
(a) from (b). The initial collision energies of Cu9− are 0.2 eV against N2O and 0.13 eV
against CO.
Cu9−
(a)
Intensity (arb. units)
Cu7O2−
Cu9O−
Cu8O−
x5
Cu9−(CO)
(b)
x5
(c)
x5
450
500
550
Mass Number (m/z)
600
Figure S2: Mass spectra obtained in the reactions of Cu11− with N2O under a multiple
collision condition (N2O pressure of 1×10−3 Torr) [panel (a)] and with a mixture of
N2O (1×10−3 Torr) and CO (5×10−3 Torr) [panel (b)]. The intensities are normalized to
the total ion intensity. Panel (c) shows a difference spectrum obtained by subtracting
(a) from (b). The initial collision energies of Cu11− are 0.2 eV against N2O and 0.13 eV
against CO.
(a)
Cu10O−
Cu10O2−
Cu11−
Cu11O−
Intensity (arb. units)
x5
Cu11−(CO)
(b)
x5
(c)
x5
600
650
700
Mass Number (m/z)
2
750
Figure S3: Mass spectra obtained in the reactions of Cun− (n = 3−16) with N2O under
single collision conditions. The N2O pressure is 1×10−4 Torr and the collision energy is
0.2 eV.
Cu3−
Cu3O
150
Cu10O−
Cu9O−
−
Cu2O−
100
Cu10−
x20
200
x20
250
500
550
600
650
Cu4−
Cu3O−
Cu11−
Cu11O−
−
Cu4O
x20
150
200
250
x20
300
600
650
700
Cu12−
Cu5−
−
x20
250
300
Cu5O−
350
Intensity (arb. units)
Intensity (arb. units)
Cu5O
x20
200
Cu6−
Cu6O−
x20
250
Cu12O−
Cu11O−
−
Cu4O
Cu3O−
750
300
350
400
650
700
750
800
−
Cu13
Cu13O−
x20
700
750
800
850
Cu14
Cu7−
−
Cu14O−
Cu7O−
Cu5O−
350
x20
x20
400
450
Cu8
800
500
850
−
900
Cu15
−
Cu8O
Cu7O−
400
450
Cu15O−
x20
500
x20
850
550
900
950
Cu16−
Cu9−
Cu9O−
Cu8O−
450
950
−
500
550
Mass Number (m/z)
1000
Cu16O−
x20
x20
900
600
3
950
1000
Mass Number (m/z)
1050
Figure S4: Mass spectra obtained in the reactions of CunO− (n = 5−12) with CO under
single collision conditions. The CO pressure is 1×10−4 Torr and the collision energy is
0.2 eV.
Cu9O−
Cu5O−
Cu5−
Cu9−
x10
x10
250
300
500
350
550
600
Cu6O−
Cu10O−
Cu6−
Cu10−
x10
350
Intensity (arb. units)
Intensity (arb. units)
x10
400
Cu7O−
600
650
Cu11O−
Cu7−
Cu11−
x10
x10
400
450
650
500
700
750
Cu12O−
Cu8O−
Cu12−
Cu8
−
x10
x10
450
500
Mass Number (m/z)
700
550
4
750
Mass Number (m/z)
800
Figure S5: CO oxidation cross sections of Cu6O− and Cu8O− as a function of the
collision energy.
3
Reaction Cross Section /ύ2
Reaction Cross Section /ύ2
1.5
Cu6O− + CO →
Cu6− + CO2
2
1
0
0.0
Cu8O− + CO →
Cu8− + CO2
1.0
0.5
0.0
0.0
0.5
1.0
Collision Energy / eV
5
0.5
1.0
Collision Energy / eV