Photocatalytic Oxidative Coupling of Methane over SrTiO3 Overlayers on Au Nanoparticles

IF 16.6 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of the American Chemical Society Pub Date : 2026-07-29 Epub Date: 2026-07-14 DOI:10.1021/jacs.6c01992

Xueyuan Wang, Pu Guo, Chenwei Ni, Xiaoju Cui, Ruotian Chen, Jianping Xiao, Nengchao Luo, Feng Wang

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引用次数: 0

Abstract

Photocatalytic oxidative coupling of methane (OCM) is a prevailing method to access multicarbon (C₂₊) hydrocarbons. However, the kinetically slow C–C coupling of the methyl radical hinders the overall methane coupling reaction and leads to overoxidation side reactions. Here we report photocatalytic OCM over SrTiO₃ supported, SrTiO₃ overlayer coated Au nanoparticles (Au@SrTiO₃). The SrTiO₃ support and overlayers capture photogenerated holes to activate the methane C–H bond. C–C coupling between the methyl radical intermediate is rate limiting and occurs with an improved selectivity of 93% over the SrTiO₃ overlayers on Au nanoparticles (NPs). The Au@SrTiO₃ catalyst is stable for more than 300 h, affording C₂H₆ with a formation rate of 155 μmol h^–1, 7 times that of Au/SrTiO₃ without SrTiO₃ overlayers. The activity is improved to 1050 μmol h^–1 with a C₂₊ selectivity of 94% by increasing Au@SrTiO₃ loading to harvest more light. These figures of merits are comparable with the benchmarking photocatalysts for OCM by elucidating the chemistry of C–C coupling sites.

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金纳米颗粒上SrTiO3覆盖层上甲烷的光催化氧化偶联。

光催化甲烷氧化偶联反应（OCM）是制备多碳（C2+）烃的常用方法。然而，甲基自由基的动力学缓慢的C-C偶联阻碍了整个甲烷偶联反应，并导致过氧化副反应。在这里，我们报道了SrTiO3负载的光催化OCM， SrTiO3覆盖的金纳米颗粒（Au@SrTiO3）。SrTiO3支架和覆盖层捕获光生成的孔以激活甲烷C-H键。甲基自由基中间体之间的C-C偶联是限速的，并且在金纳米颗粒（NPs）上的SrTiO3覆盖层上的选择性提高了93%。Au@SrTiO3催化剂在300 h以上稳定生成C2H6，生成速率为155 μmol h-1，是无SrTiO3包覆层Au/SrTiO3的7倍。通过增加Au@SrTiO3负载获得更多的光，将活性提高到1050 μmol h-1， C2+选择性为94%。通过阐明C-C偶联位点的化学性质，这些优点与OCM的基准光催化剂相当。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Journal of the American Chemical Society 化学-化学综合

CiteScore

24.40

自引率

6.00%

发文量

2398

审稿时长

1.6 months

期刊介绍： The flagship journal of the American Chemical Society, known as the Journal of the American Chemical Society (JACS), has been a prestigious publication since its establishment in 1879. It holds a preeminent position in the field of chemistry and related interdisciplinary sciences. JACS is committed to disseminating cutting-edge research papers, covering a wide range of topics, and encompasses approximately 19,000 pages of Articles, Communications, and Perspectives annually. With a weekly publication frequency, JACS plays a vital role in advancing the field of chemistry by providing essential research.