Selective Photocatalytic Oxidation of Methane to Methanol by Constructing a Rapid O2 Conversion Pathway over Au-Pd/ZnO

被引：41

作者：

Zhou, Qiang ^{[1
,2
]}

Tan, Xiaojie ^{[1
,2
]}

Wang, Xinyu ^{[1
,2
]}

Zhang, Qinhua ^{[1
,2
]}

Qi, Chong ^{[1
,2
]}

Yang, Hao ^{[1
,2
]}

He, Zhengqiu ^{[1
,2
]}

Xing, Tao ^{[3
]}

Wang, Mingqing ^{[3
]}

Wu, Mingbo ^{[1
,2
]}

Wu, Wenting ^{[1
,2
]}

机构：

[1] China Univ Petr East China, Coll Chem & Chem Engn, State Key Lab Heavy Oil Proc, Qingdao 266580, Peoples R China

[2] China Univ Petr East China, Inst New Energy, Qingdao 266580, Peoples R China

[3] ShanDong Energy Grp CO LTD, Natl Engn Res Ctr Coal Gasificat & Coal Based Adv, Jinan 250101, Peoples R China

来源：

ACS CATALYSIS | 2024年 / 14卷 / 02期

基金：

中国国家自然科学基金;

关键词：

photocatalysis; methaneoxidation; radicalregulation; oxygen activation; nanomaterial; BOND ACTIVATION; OXYGEN; PD; H2O2; CH4;

D O I：

10.1021/acscatal.3c04374

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

Photocatalytic oxidation of methane to methanol is an attractive process under mild conditions, nevertheless confronting significant challenges in achieving high conversion and selectivity simultaneously. Herein, we propose a strategy for the direct and rapid generation of hydroxyl radicals ((OH)-O-center dot) from O-2 (O-2 -> *OOH -> (OH)-O-center dot) by rational design of Au-Pd/ZnO photocatalyst, skipping water-soluble H2O2 and avoiding H2O2 diffusion. For photocatalytic methane oxidation at ambient temperature, the yield and selectivity of CH3OH over the optimized 1.0% AuPd0.5/ZnO catalyst were as high as 81.0 mu mol<middle dot>h(-1) and 88.2%, respectively, exceeding that of most reported systems. The formation of Au-Pd alloys could improve the O-2 adsorption and the cleavage of the O-O bond in *OOH, facilitating the efficient direct formation of (OH)-O-center dot and increasing the CH3OH yield and selectivity. This work provides some guidance for the delicate design of composite photocatalysts for efficient selective photocatalytic methane oxidation and O-2 utilization.

引用

页码：955 / 964

页数：10

共 52 条

[1] Aqueous Au-Pd colloids catalyze selective CH4 oxidation to CH3OH with O2 under mild conditions [J].