Electrochemically Promoted Activation of Light Alkanes at Ambient Conditions

IF 16.9 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Angewandte Chemie International Edition Pub Date : 2025-04-22 DOI:10.1002/anie.202507417
Wenxuan Liu, Hsien-Chin Li, Chunsong Li, Wei-Sen Chen, Haochen Zhang, Bingjun Xu, Mu-Jeng Cheng, Qi Lu
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Abstract

The electrochemical activation of light alkanes into value-added products represents a promising pathway for sustainable chemical synthesis and the storage of renewable energy. In this study, we introduce an electrochemically promoted system that employs copper plates as electrode and oxygen as oxidant, capable of converting ethane into ethylene and acetic acid with production rates of 6.9 and 6.2 µmol·cm−2Cu·h−1, respectively, with a combined selectivity exceeding 92%, under ambient conditions. Additionally, this system can convert propane to propylene at a rate of 11.6 µmol·cm−2Cu·h−1, with selectivity reaching up to 86%. A 10 h run with ethane demonstrates consistent production of ethylene and acetic acid, with a sustained selectivity above 96%, and achieves an acetic acid concentration of 19 mM. In situ spectroscopic analysis reveals the active surface and a critical reaction intermediate. Combining with partial pressure dependence study and density functional theory (DFT) calculations, we propose a potential reaction mechanism involving the competitive adsorption of oxygen and alkane producing an alkyl group as a key reaction step in the reaction process.

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在环境条件下电化学促进轻烷的活化
轻烷烃的电化学活化成增值产品代表了可持续化学合成和可再生能源储存的一个有前途的途径。在本研究中,我们介绍了一种电化学促进系统,该系统以铜板为电极,氧为氧化剂,能够在环境条件下将乙烷转化为乙烯和乙酸,产率分别为6.9和6.2µmol·cm - 2Cu·h - 1,总选择性超过92%。此外,该体系能以11.6µmol·cm−2Cu·h−1的速率将丙烷转化为丙烯,选择性高达86%。用乙烷运行10小时,乙烯和乙酸的产量一致,选择性持续高于96%,乙酸浓度达到19 mM。原位光谱分析揭示了活性表面和关键反应中间体。结合分压依赖性研究和密度泛函理论(DFT)计算,我们提出了一种潜在的反应机理,其中氧和烷烃的竞争吸附产生烷基是反应过程中的关键反应步骤。
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来源期刊
CiteScore
26.60
自引率
6.60%
发文量
3549
审稿时长
1.5 months
期刊介绍: Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.
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