Reactions of gold cluster cations <tex>$Au_{n}^{+}$</tex> (n = 112) with <tex>$H_{2}S$</tex> and <tex>$H_{2}$</tex>Reactions of gold cluster cations <tex>$Au_{n}^{+}$</tex> (n = 112) with <tex>$H_{2}S$</tex> and <tex>$H_{2}$</tex>
Faculty of Sciences. Chemistry

article

2003New York, N.Y., 2003

Chemistry

The journal of chemical physics. - New York, N.Y.

118(2003):17, p. 7808-7816

0021-9606

000182276100011

E

Dutch (dut)

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.

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