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Ag/AgCl@SiO上甲烷选择性光催化有氧氧化制一氧化碳

Selective photocatalytic aerobic oxidation of methane into carbon monoxide over Ag/AgCl@SiO.

作者信息

Zhai Jianxin, Zhou Baowen, Wu Haihong, Jia Shuaiqiang, Chu Mengen, Han Shitao, Xia Wei, He Mingyuan, Han Buxing

机构信息

Shanghai Key Laboratory of Green Chemistry and Chemical Processes, School of Chemistry and Molecular Engineering, East China Normal University Shanghai 200062 China

Key Laboratory for Power Machinery and Engineering of Ministry of Education, School of Mechanical Engineering, Shanghai Jiao Tong University Shanghai 200240 China

出版信息

Chem Sci. 2022 Mar 30;13(16):4616-4622. doi: 10.1039/d2sc01140a. eCollection 2022 Apr 20.

Abstract

Design of active catalysts for chemical utilization of methane under mild conditions is of great importance, but remains a challenging task. Here, we prepared a Ag/AgCl with SiO coating (Ag/AgCl@SiO) photocatalyst for methane oxidation to carbon monoxide. High carbon monoxide production (2.3 μmol h) and high selectivity (73%) were achieved. SiO plays a key role in the superior performance by increasing the lifetime of the photogenerated charge carriers. Based on a set of semi infrared spectroscopy, electron paramagnetic resonance, and electronic property characterization studies, it is revealed that CH is effectively and selectively oxidized to CO by the formation of singlet O the key intermediate of COOH*. Further study showed that the Ag/AgCl@SiO catalyst could also drive valuable conversion using real sunlight under ambient conditions. As far we know, this is the first work on the application of SiO modified Ag/AgCl in the methane oxidation reaction.

摘要

在温和条件下设计用于甲烷化学利用的活性催化剂非常重要,但仍然是一项具有挑战性的任务。在此,我们制备了一种具有SiO涂层的Ag/AgCl(Ag/AgCl@SiO)光催化剂用于将甲烷氧化为一氧化碳。实现了高一氧化碳产量(2.3 μmol/h)和高选择性(73%)。SiO通过延长光生电荷载流子的寿命在优异性能中起关键作用。基于一系列红外光谱、电子顺磁共振和电子性质表征研究,揭示了CH通过形成单线态O(COOH*的关键中间体)被有效且选择性地氧化为CO。进一步研究表明,Ag/AgCl@SiO催化剂在环境条件下也能利用真实阳光驱动有价值的转化。据我们所知,这是关于SiO修饰的Ag/AgCl在甲烷氧化反应中应用的首次工作。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/16d8/9020177/0b1648fd0039/d2sc01140a-f1.jpg

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