Selective photocatalytic oxidation of methane to C1 oxygenates by regulating sizes and facets over Au/ZnO  

作　　者：Qiang Zhou Xinyu Wang Xiaojie Tan Qinhua Zhang Hao Yang Tao Xing Mingqing Wang Mingbo Wu Wenting Wu 

机构地区：[1]State Key Laboratory of Heavy Oil Processing,College of Chemistry and Chemical Engineering&Institute of New Energy,China University of Petroleum(East China),Qingdao 266580,China [2]National Engineering Research Center of Coal Gasification and Coal-Based Advanced Materials,ShanDong Energy Group CO.LTD,Jinan 250101,China

出　　处：《Nano Research》2024年第5期3810-3818,共9页纳米研究（英文版）

基　　金：supported by the National Key Research and Development Program of China(No.2019YFA0708700);the National Natural Science Foundation of China(Nos.22322815,22179146,51672309,51172285,51372277);the Major Scientific and Technological Innovation Project of Shandong Province(No.2020CXGC010402);the Fundamental Research Funds for Central Universities(No.18CX07009A);YanKuang Group Co.,Ltd.(No.YKZB2020-167);the Young Taishan Scholar Program of Shandong Province(No.tsqn20182027);Taishan Scholar Project(No.ts201712020);the Technological Leading Scholar of 10000 Talent Project(No.W03020508).

摘　　要：Photocatalytic oxidation of methane to value-added chemicals is a promising process under mild conditions,nevertheless confronting great challenges in efficiently activating C-H bonds and inhibiting over-oxidation.Herein,we propose a comprehensive strategy for the selective generation of reactive oxygen species(ROS)by regulating the sizes and facets of Au nanoparticles loaded on ZnO.For photocatalytic methane oxidation at ambient temperature,a high oxygenates yield of 36.4 mmol·g^(-1)·h^(-1) with a nearly 100%selectivity has been achieved over the optimized 1.0%Au/ZnO-9.6(1%Au with(111)facet and 9.6 nm size on ZnO)photocatalyst,exceeding most reported literatures.Mechanism investigations reveal that 1.0%Au/ZnO-9.6 with the medium size and Au(111)facet guarantees the favourable formation of superoxide radicals(·OOH)through mild oxygen reduction,ultimately leading to excellent photocatalytic methane oxidation performance.This work provides some guidance for the delicate design of photocatalysts for efficient photocatalytic methane oxidation and oxygen utilization.

关 键 词：photocatalysis methane oxidation radical regulation oxygen activation NANOMATERIAL 

分 类 号：O64[理学—物理化学]