Regulation of O2 activation pathway boosts efficient photocatalytic methane oxidation to methanol

被引:3
作者
Zhou, Qiang [1 ]
Wan, Yi [1 ]
Wang, Xinyu [1 ]
Zhang, Qinhua [1 ]
Zhang, Haonan [1 ]
Qi, Chong [1 ]
Liu, Ziyu [1 ]
Yang, Hao [1 ]
Xing, Tao [2 ]
Wang, Mingqing [2 ]
Wu, Mingbo [1 ]
Wu, Wenting [1 ]
机构
[1] China Univ Petr East China, Inst New Energy, Coll Chem & Chem Engn, State Key Lab Heavy Oil Proc, Qingdao 266580, Shandong, Peoples R China
[2] ShanDong Energy Grp CO LTD, Natl Engn Res Ctr Coal Gasificat & Coal Based Adv, Jinan 250101, Shandong, Peoples R China
基金
中国国家自然科学基金;
关键词
Photocatalysis; Methane oxidation; Radical regulation; Oxygen activation; Oxygen vacancy; ROOM-TEMPERATURE; CONVERSION; OXYGEN; AU; O-2; CH4;
D O I
10.1016/j.seppur.2024.129064
中图分类号
TQ [化学工业];
学科分类号
0817 ;
摘要
Photocatalytic oxidation of methane to methanol is a promising process under mild conditions, nevertheless confronting great challenges in achieving high yield and selectivity of methanol simultaneously. Herein, we propose a strategy for the proper amount of hydroxyl radicals (center dot OH) generation from O2 by rational design of Au nanoparticles and oxygen vacancies (OVs) co-decorated ZnO photocatalysts. For photocatalytic methane oxidation at ambient temperature, a high CH3OH yield of 6.3 mmol center dot g- 1 center dot h- 1 with a nearly 100 % selectivity has been achieved over the optimized Au2.5-def-ZnO (2.5 wt% Au and OVs co-decorated ZnO) photocatalyst, exceeding most reported literatures. Mechanism investigations revealed that Au nanoparticles and OVs synergistically promoted charge separation, improved the adsorption and activation of CH4 and O2, facilitating the selective generation of center dot OH from O2. Combined with the aqueous phase system, the over-oxidation of CH3OH was effectively inhibited, thereby achieving high yield and high selectivity of CH3OH simultaneously. This work provides some guidance for the design of high-performance photocatalysts for photocatalytic selective oxidation of methane to methanol.
引用
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页数:13
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