甲烷
光催化
甲醇
光化学
催化作用
甲烷厌氧氧化
选择性
氧化还原
材料科学
可见光谱
氧气
激发态
等离子体子
化学
量子效率
合理设计
无机化学
反应机理
能量转换效率
等离子纳米粒子
反应速率
纳米技术
工作(物理)
电子
部分氧化
人工光合作用
作者
Bin Li,Yangyang Zhu,Ji Bian,Ziqing Zhang,Liqiang Jing
标识
DOI:10.1021/acscatal.6c03797
摘要
Abstract Solar-driven direct oxidation of methane to methanol with WO3 offers a promising avenue for methane utilization, yet the activation of O2 remains a challenge. Here, a FeOx–Au co-modified urchin-like WO3-x with surface oxygen vacancies is fabricated by a one-step redox co-deposition protocol for selective methane conversion to methanol. An impressive CH3OH production rate of 5.4 mmol g–1 h–1 (apparent quantum efficiency of 12.1% at the plasmonic wavelength of 660 nm) with a near unity selectivity (ca. 95%) is achieved, ranking among the top in the WO3-based photocatalysts reported to date under comparable reaction conditions. Experimental results unravel that the excited electrons especially for plasmonic hot ones on WO3-x could be rapidly extracted by the Au and then transferred to FeOx for activating O2 to generate •O2– radicals. In parallel, the generated holes participate in attacking methane for producing methyl radicals. This work proposes a strategy for the rational design of plasmonic photocatalysts for selective CH4 photo-oxidation.
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