三氧化钨
催化作用
光催化
甲醇
甲烷
脱氢
钨
化学
光化学
吸附
无机化学
材料科学
化学工程
纳米技术
物理化学
有机化学
工程类
作者
Yi Zeng,Zhiyuan Tang,Xingyang Wu,Anhua Huang,Xin Luo,Guo Qin Xu,Yongfa Zhu,Song Ling Wang
标识
DOI:10.1016/j.apcatb.2021.120919
摘要
Atomic-scale metals as active center have been widely investigated for efficient photocatalysis. Understanding the specific electronic structure of atomic-scale center is of profound fundamental importance for superior catalytic performance. Here, we report an atomically dispersed gold on tungsten trioxide (Au1/WO3) catalyst for photocatalytic oxidation of methane toward value-added methanol. The Au1 species reveal a specific tip-enhanced local electrons field which favors the C-H dehydrogenation of methane and thus form methanol (up to 589 µmol g−1 h−1). Both experimental and theoretical results demonstrate such tip-enhanced effect enhance the catalytic activity of methane oxidation. The theoretical calculations further reveal a lower adsorption energy of product methanol on Au1, in contrast to Au particles, which suppresses the overoxidation of methanol, and thus promotes its selectivity. Establishing the relationship between electronic density and catalytic activity may create a platform for designing efficient atomic-scale catalysts for C1 catalysis and green chemistry.
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