A Broad Range of Aromatic Carboxylic Acids for Photocatalytic Methane Oxidation.

IF 27.4 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Advanced Materials Pub Date : 2025-06-16 DOI:10.1002/adma.202504866

Xiangyang Wang,Guohao Jiang,Xuefeng He,Qiuling Wang,Zhaomin Su,Xue Wang,Cheng Wang

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引用次数: 0

Abstract

Photocatalytic methane (CH₄) activation under mild conditions presents a sustainable strategy for converting methane into valuable chemicals. This study introduces a versatile class of conjugated aromatic carboxylic acids as efficient, metal-free photocatalysts for CH₄ oxidation in sodium chloride-trifluoroacetic acid (NaCl-TFA) media. Spectroscopic analysis and machine learning using spectroscopic features further elucidate key structural and electronic factors influencing catalytic activity, offering predictive insights for designing high-performance photocatalysts. The carboxyl group is important in generating electron-deficient carboxyl (RC(═O)O•) or carboperoxyl radicals (RC(═O)OO•), enabling selective hydrogen atom transfer (HAT) for CH₄ functionalization. Mechanistic investigations indicate the role of acyl chloride intermediates in enhancing reactivity. This work highlights the potential of aromatic carboxylic acids to address the challenges of methane functionalization, paving the way for greener chemical transformations and the utilization of inert feedstocks in sustainable chemistry.

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用于光催化甲烷氧化的各种芳香羧酸。

在温和条件下光催化甲烷（CH₄）活化为甲烷转化为有价值的化学品提供了一种可持续的策略。本研究介绍了一种多功能的共轭芳香羧酸类，作为氯化钠-三氟乙酸（NaCl-TFA）介质中氯化氯化钠氧化的高效、无金属光催化剂。光谱分析和利用光谱特征的机器学习进一步阐明了影响催化活性的关键结构和电子因素，为设计高性能光催化剂提供了预测性见解。羧基在生成缺电子羧基（RC(= O)O•）或碳过氧自由基（RC(= O)OO•）中是重要的，使得选择性氢原子转移（HAT）能够实现CH₄官能化。机理研究表明酰基氯中间体在提高反应活性方面的作用。这项工作强调了芳香羧酸在解决甲烷功能化挑战方面的潜力，为绿色化学转化和可持续化学中惰性原料的利用铺平了道路。

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

Advanced Materials 工程技术-材料科学：综合

CiteScore

43.00

自引率

4.10%

发文量

2182

审稿时长

2 months

期刊介绍： Advanced Materials, one of the world's most prestigious journals and the foundation of the Advanced portfolio, is the home of choice for best-in-class materials science for more than 30 years. Following this fast-growing and interdisciplinary field, we are considering and publishing the most important discoveries on any and all materials from materials scientists, chemists, physicists, engineers as well as health and life scientists and bringing you the latest results and trends in modern materials-related research every week.