金红石
甲烷
氧气
甲烷厌氧氧化
材料科学
化学工程
环境化学
化学
矿物学
有机化学
工程类
作者
Yuemiao Lai,Ruimin Wang,Yi Zeng,Fangliang Li,Xiao Chen,Tao Wang,Hongjun Fan,Qing Guo
出处
期刊:JACS Au
[American Chemical Society]
日期:2024-03-26
标识
DOI:10.1021/jacsau.3c00771
摘要
Understanding the microkinetic mechanism underlying photocatalytic oxidative methane (CH4) conversion is of significant importance for the successful design of efficient catalysts. Herein, CH4 photooxidation has been systematically investigated on oxidized rutile(R)-TiO2(110) at 60 K. Under 355 nm irradiation, the C–H bond activation of CH4 is accomplished by the hole-trapped dangling OTi– center rather than the hole-trapped Ob– center via the Eley–Rideal reaction pathway, producing movable CH3• radicals. Subsequently, movable CH3• radicals encounter an O/OH species to form CH3O/CH3OH species, which could further dissociate into CH2O under irradiation. However, the majority of the CH3• radical intermediate is ejected into a vacuum, which may induce radical-mediated reactions under ambient conditions. The result not only advances our knowledge about inert C–H bond activation but also provides a deep insight into the mechanism of photocatalytic CH4 conversion, which will be helpful for the successful design of efficient catalysts.
科研通智能强力驱动
Strongly Powered by AbleSci AI