期刊
ACS CATALYSIS
卷 10, 期 23, 页码 14318-14326出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.0c04329
关键词
methane oxidation; methanol; photocatalysis; titanium dioxide; dual cocatalysts; nanometals; cobalt oxide
资金
- Photo-excitonix Project in Hokkaido University
- National Natural Science Foundation of China [21633004, 51872091, 51902121]
- Hundred Talents Program of Hebei Province [E2018050013]
- Fundamental Research Funds for the Central Universities of China [2662018QD011]
- Natural Science Foundation of Hubei Province [2019CFB322]
- JSPS KAKENHI [JP18H02065]
Direct and selective oxidation of CH4 with dioxygen to methanol is a dream reaction in modern catalysis yet remains a great challenge. Here, we report that TiO2 loaded with dual cocatalysts, that is, nanometals and cobalt oxide (CoOx) nanoclusters, is capable of selectively catalyzing CH4 to CH3OH at room temperature under photoexcitation using abundant and inexpensive O-2 as an oxidant. The best activity for the formation of the primary products, CH3OOH and CH3OH, is up to 50.8 pmol for 2 h with 95% selectivity. Mechanistic studies elucidate that the superior activity and selectivity result from the synergistic effect of nanometals and CoOx. Nanometals enhance CH4 conversion by promoting the separation of the photoexcited electron and the reduction of O-2. The CoOx mediates a mild CH4 oxidation process by suppressing the formation of highly oxidative (OH)-O-center dot radicals that can further oxidize CH3OH to HCHO and CO2, thereby preserving a high selectivity toward oxygenated products. This work provides a prototype in designing efficient photocatalysts for selective oxidation of CH4 to CH3OH with O-2 under mild conditions.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据