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Ultrasmall Au10 clusters anchored on pyramid-capped rectangular TiO2 for olefin oxidation

Journal 2016 · IF 8.893 · 9(4): 1182-1192 · 发表于 2016 年 3 月 11 日
作者: Li Lixiong,Huang Shuangshuang,Song Jianjun,Yang Nating,Liu Jingwei,Chen Yuyun,Sun Yuhan,Jin Rongchao,Zhu Yan
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摘要

Ultrasmall Au 10 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 Au 10 on the catalytic oxidation, a TiO 2 charge carrier was chosen as the substrate to anchor Au 10 for olefin oxidation. Au 10 supported on TiO 2 -RP (RP = pyramid-capped columnar structure) exhibited superior catalytic activity to Au 10 /TiO 2 nanotubes and Au 10 /P25. In addition, the supported Au 10 clusters gave rise to higher activity than supported Au 20 , Au 144 clusters, and 5 nm Au nanocrystals. The superior catalytic ability of Au 10 /TiO 2 -RP arises from the charge/discharge effect of the Au 10 /TiO 2 -RP interface, which effectively improves the formation of active oxygen species on electron-rich gold atoms at the terminal position of Au 10 , and promotes the activation of olefin C=C bonds on the electron-deficient gold atoms of Au 10 .