具有缺陷结构的Au负载ZnSn-LDH通过氧定向活化实现甲烷选择性光催化氧化偶联-CSCIED科技核心评价数据库-手机版

具有缺陷结构的Au负载ZnSn-LDH通过氧定向活化实现甲烷选择性光催化氧化偶联

Selective photocatalytic oxidative coupling of methane via directional activation of oxygen over Au-loaded ZnSn-LDH with defect structure

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DOI	10.1016/j.apcatb.2024.124670
刊名	Applied Catalysis B: Environment and Energy
年，卷(期)	2024, 361()
作者	张金宇, 冯晓燕, 李莉 * , 王萍, 梁军 *,
作者单位	宁夏大学
摘要	甲烷选择性光催化氧化偶联反应在将低成本原料转化为C2产物方面具有巨大潜力。然而，如何通过催化剂设计提升光催化OCM活性，并深入理解OCM过程中的反应物活化机制仍面临挑战。本研究合成了具有氧空位的Au-ZnSn-LDH，实现了以O2为氧化剂的高效甲烷选择性氧化。优化后的复合催化剂表现出2666 μmol·g?1·h?1的乙烷产率和76.8%的选择性。研究结果表明，ZnSn-LDH表面的氧（可能吸附于氧空位）在金助催化剂的辅助下，为O2活化为O2?提供了位点。O2?可由O2转化生成，在光激发下能选择性地促进甲烷C-H键活化，展现理想的反应活性。金助催化剂在促进甲基转移、加速C-C偶联以生成主要产物乙烷，并避免不利的过度氧化反应方面起着关键作用。
Abstract	The selective photocatalytic oxidative coupling of methane (OCM) holds great potential in converting low-cost feedstock into C2 products. However, the challenge lies in improving the photocatalytic OCM activity through catalyst design and gaining a deeper understanding of reactant activation in the OCM process. Here, we synthesized Au-ZnSn-LDH with oxygen vacancies to achieve efficient selective oxidation of methane using O2. The optimal hybrid exhibits a C2H6 yield of 2666 μmol g? 1 h? 1 and 76.8 % selectivity. Our findings showed that the oxygen within the surface of ZnSn-LDH (possibly from adsorption at Ov vacancy sites) provides sites for the evolution of O2 to O2 with assistance from Au cocatalyst. More O2 could be generated from O2 provides a desired reactivity to selectively promote selective C? H activation of CH4 under photoexcitation. The Au cocatalyst plays crucial roles in facilitating the methyl transfer and promoting C? C coupling to produce C2H6 as the main product while avoiding undesirable overoxidation.
关键词	Au负载ZnSn层状双氢氧化物;光催化;C-H键活化;甲烷氧化偶联;乙烷
KeyWord	Au-ZnSn-LDH;Photocatalysis;C-H activation;Oxidative methane coupling;C2H6
基金项目
页码	1-8

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张金宇, 冯晓燕, 李莉 * , 王萍, 梁军 *. 具有缺陷结构的Au负载ZnSn-LDH通过氧定向活化实现甲烷选择性光催化氧化偶联 [J]. Applied Catalysis B: Environment and Energy. 2024; 361; (). 1 - 8.

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