利用非过渡金属电极,通过CO2·−中间体对芳香羧酸进行一般的电化学CO2固定

IF 9.7 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Baijing Wu, Xiaoxue Luo, Hongliang Fan, Minhua Shao, Cunpu Li, Zidong Wei
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引用次数: 0

摘要

二氧化碳固定对于减少温室效应和提高清洁能源的使用具有重要意义。虽然最近的研究重点是将二氧化碳转化为液体燃料,但直接固定为芳香羧酸等高价值化合物提供了另一种途径。在此,我们报道了一种利用非过渡金属石墨电极通过CO2·−中间体对芳香羧酸进行一般电化学CO2固定的方法。与传统的芳香族自由基机制不同的是,在本研究中,CO2会在石墨电极上获得电子生成CO2·−,CO2·−会进一步攻击芳香族卤化物,通过芳香族亲核取代机制得到所需的芳香族羧酸。由于CO2·−作为一般中间体,各种芳香族化合物可以羰基化,而不需要特定的催化设计来激活芳香族卤化物。此外,得益于CO2·−亲核试剂,与传统方法相比,只能得到ipso产物。该方法为将温室气体CO2转化为有价值的芳香族羧酸提供了一种灵活的方法,在药物化学、生物化学和聚合物化学等领域都有应用。因此,它具有进一步实现碳中和和绿色化学目标的潜力。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
A general electrochemical CO2 fixation to aromatic carboxylic acids via the CO2·− intermediate using a non-transition metal electrode

CO2 fixation is important for reducing the greenhouse effect and improving clean energy use. While recent studies focus on converting CO2 to liquid fuels, direct fixation into high-value compounds like aromatic carboxylic acids provides an alternative path. Herein, we report a general electrochemical CO2 fixation to aromatic carboxylic acids via the CO2·− intermediate using a non-transition metal graphite electrode. Different from the conventional aromatic radical mechanism, in this report, CO2 will gain electrons on the graphite electrode to generate CO2·−, which will further attack aromatic halides to obtain the desired aromatic carboxylic acid via an aromatic nucleophilic substitution mechanism. As CO2·− acts as the general intermediate, various aromatic compounds can be carbonylated without the need for a specific catalytic design to activate the aromatic halides. Furthermore, benefit from the CO2·− nucleophile, only the ipso-products can be obtained compared with the conventional approaches. This method offers a flexible way to convert the greenhouse gas CO2 into valuable aromatic carboxylic acids, which have applications in pharmaceutical chemistry, biochemistry and polymer chemistry. Therefore, it holds the potential for furthering the objectives of carbon neutrality and green chemistry.

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来源期刊
Science China Chemistry
Science China Chemistry CHEMISTRY, MULTIDISCIPLINARY-
CiteScore
14.40
自引率
7.30%
发文量
3787
审稿时长
2.2 months
期刊介绍: Science China Chemistry, co-sponsored by the Chinese Academy of Sciences and the National Natural Science Foundation of China and published by Science China Press, publishes high-quality original research in both basic and applied chemistry. Indexed by Science Citation Index, it is a premier academic journal in the field. Categories of articles include: Highlights. Brief summaries and scholarly comments on recent research achievements in any field of chemistry. Perspectives. Concise reports on thelatest chemistry trends of interest to scientists worldwide, including discussions of research breakthroughs and interpretations of important science and funding policies. Reviews. In-depth summaries of representative results and achievements of the past 5–10 years in selected topics based on or closely related to the research expertise of the authors, providing a thorough assessment of the significance, current status, and future research directions of the field.
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