石墨烯
催化作用
甲醇
Atom(片上系统)
选择性
甲烷
材料科学
化学
非阻塞I/O
光化学
无机化学
纳米技术
有机化学
计算机科学
嵌入式系统
作者
Fei Ying,Bo Zhao,Zhixin Ren,Jing Xie
标识
DOI:10.1021/acs.jpcc.3c04213
摘要
Inspired by the excellent performance of NiO+ in converting CH4 to CH3OH in the gas phase and the efficiency of single-atom catalysts, we constructed a Ni–O active site on single-vacant (SV) graphene by using O3/N2O as the oxidant. Quantum chemistry calculations predict Ni/SV-graphene to be a potential catalyst for CH4-to-CH3OH conversion, outperforming Pd or Pt/SV-graphene in both the activity and selectivity. The radical pathway is favored, and the C–H bond activation is the rate-determining step, during which an electron is transferred from CH4 to the O-atom of OM/SV-graphene and pushes an electron from σM–O orbital to σM–O*. The ONi/SV-graphene has smaller σM–O* to σM–O energy gap than its Pd/Pt counterparts, thus more readily transferring the electron to activate the C–H bond, making it the best catalyst. In addition, Ni/SV-graphene is capable of recycling and avoiding overoxidizing of methanol. This study provides theoretical insights into developing efficient noble-metal-free catalysts for direct CH4-to-CH3OH conversion.
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