|
Title
|
|
|
|
Reactions of gold cluster cations (n = 112) with and
| |
|
Author
|
|
|
|
| |
|
Abstract
|
|
|
|
| The reactions of gold cluster cations Aun+ (n = 112) with H2S and H2 have been studied using Fourier-transform ion-cyclotron resonance (FTICR) mass spectrometry. The cluster cations were produced by laser ablation of a gold rod in He atmosphere, and their reactions were observed at room temperature and low total pressures of 10−710−5 Torr. Initial products of the reactions with H2S were mainly AuSH+ for n = 2, AunS+ for n = 48 and 10, and AunSH2+ for n = 9, 11, and 12. No reactions of Au+ and Au3+ with H2S were observed. Even n cluster cations were more reactive than adjacent odd n clusters. The particularly low reactivity at n = 1, 3, 9, and 11 is consistent with the low ionization potential of Aun and the weak binding energy of Aun+Au. Further sulfuration reactions of AunS+ proceeded to give AunSm+ and finally stopped at AunSm+xH2+ when H2 release did not occur. The maximum number of sulfur atoms m+x increased with the cluster size up to n = 8, while the sulfuration reaction stopped at early stages for n ≥ 9. In another series of experiments, no reaction of Aun+ (n = 112) with H2 gas pulses introduced into the FTICR cell was observed. To investigate the stability of gold hydride clusters, laser ablation of gold in a H2/He mixture was performed. The hydride cluster cations AunHm+ were produced for n = 17, while bare Aun+ clusters were the main products for n ≥ 8. There is a distinct border between n = 7 and 8, as the structure of Aun+ changes from planar for n ⩽ 7 to three-dimensional for n ≥ 8, suggesting the stability of hydride cluster cations with planar gold frameworks. |
| |
|
Language
|
|
|
|
Dutch
| |
|
Source (journal)
|
|
|
|
The journal of chemical physics. - New York, N.Y.
| |
|
Publication
|
|
|
|
New York, N.Y.
:
2003
| |
|
ISSN
|
|
|
|
0021-9606
| |
|
DOI
|
|
|
|
10.1063/1.1564057
| |
|
Volume/pages
|
|
|
|
118
:17
(2003)
, p. 7808-7816
| |
|
ISI
|
|
|
|
000182276100011
| |
|
Full text (Publisher's DOI)
|
|
|
|
| |
|