催化作用
钯
铈
酒精氧化
化学
氧化铈
苯甲醛
酒
星团(航天器)
金属
选择性
透射电子显微镜
氧化物
无机化学
有机化学
材料科学
纳米技术
计算机科学
程序设计语言
作者
Pingyu Xin,Jia Li,Yu Xiong,Xi Wu,Juncai Dong,Wenxing Chen,Yu Wang,Lin Gu,Jun Luo,Hongpan Rong,Chen Chen,Qing Peng,Dingsheng Wang,Yadong Li
标识
DOI:10.1002/anie.201801103
摘要
The active species in supported metal catalysts are elusive to identify, and large quantities of inert species can cause significant waste. Herein, using a stoichiometrically precise synthetic method, we prepare atomically dispersed palladium-cerium oxide (Pd1 /CeO2 ) and hexapalladium cluster-cerium oxide (Pd6 /CeO2 ), as confirmed by spherical-aberration-corrected transmission electron microscopy and X-ray absorption fine structure spectroscopy. For aerobic alcohol oxidation, Pd1 /CeO2 shows extremely high catalytic activity with a TOF of 6739 h-1 and satisfactory selectivity (almost 100 % for benzaldehyde), while Pd6 /CeO2 is inactive, indicating that the true active species are single Pd atoms. Theoretical simulations reveal that the bulkier Pd6 clusters hinder the interactions between hydroxy groups and the CeO2 surface, thus suppressing synergy of Pd-Ce perimeter.
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