UltrasmaU Au10 clusters have a unique electronic structure and can act as a charge reservoir to donate electrons or accept charges. This is particularly important for catalysis, since it leads to facile charge transfe...UltrasmaU Au10 clusters have a unique electronic structure and can act as a charge reservoir to donate electrons or accept charges. This is particularly important for catalysis, since it leads to facile charge transfer across the interface between the gold species and the oxide substrate. To determine the electronic and structural effects of Au10 on the catalytic oxidation, a TiO2 charge carrier was chosen as the substrate to anchor Au10 for olefin oxidation. Au10 supported on TiO2-RP （RP = pyramid-capped columnar structure） exhibited superior catalytic activity to Au10/TiO2 nanotubes and Au10/P25. In addition, the supported Au10 clusters gave rise to higher activity than supported Au20, Au144 clusters, and 5 nm Au nanocrystals. The superior catalytic ability of Au^0fFiO2-RP arises from the charge/discharge effect of the Au10/TiO2-RP interface, which effectively improves the formation of active oxygen species on electron-rich gold atoms at the terminal position of Au10, and promotes the activation of olefin C--C bonds on the electron-deficient gold atoms of Au10.展开更多
基金We are grateful for financial support by the National Natural Science Foundation of China （No. 21273151）, and Hundred Talent Program of Chinese Academy of Sciences. Y. Z. acknowledges support by Ministry of Education for returned overseas Chinese scholars.
文摘UltrasmaU Au10 clusters have a unique electronic structure and can act as a charge reservoir to donate electrons or accept charges. This is particularly important for catalysis, since it leads to facile charge transfer across the interface between the gold species and the oxide substrate. To determine the electronic and structural effects of Au10 on the catalytic oxidation, a TiO2 charge carrier was chosen as the substrate to anchor Au10 for olefin oxidation. Au10 supported on TiO2-RP （RP = pyramid-capped columnar structure） exhibited superior catalytic activity to Au10/TiO2 nanotubes and Au10/P25. In addition, the supported Au10 clusters gave rise to higher activity than supported Au20, Au144 clusters, and 5 nm Au nanocrystals. The superior catalytic ability of Au^0fFiO2-RP arises from the charge/discharge effect of the Au10/TiO2-RP interface, which effectively improves the formation of active oxygen species on electron-rich gold atoms at the terminal position of Au10, and promotes the activation of olefin C--C bonds on the electron-deficient gold atoms of Au10.
