{"title":"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","authors":"Baijing Wu, Xiaoxue Luo, Hongliang Fan, Minhua Shao, Cunpu Li, Zidong Wei","doi":"10.1007/s11426-025-2639-8","DOIUrl":null,"url":null,"abstract":"<div><p>CO<sub>2</sub> fixation is important for reducing the greenhouse effect and improving clean energy use. While recent studies focus on converting CO<sub>2</sub> to liquid fuels, direct fixation into high-value compounds like aromatic carboxylic acids provides an alternative path. Herein, we report a general electrochemical CO<sub>2</sub> fixation to aromatic carboxylic acids via the CO<sub>2</sub><sup>·−</sup> intermediate using a non-transition metal graphite electrode. Different from the conventional aromatic radical mechanism, in this report, CO<sub>2</sub> will gain electrons on the graphite electrode to generate CO<sub>2</sub><sup>·−</sup>, which will further attack aromatic halides to obtain the desired aromatic carboxylic acid via an aromatic nucleophilic substitution mechanism. As CO<sub>2</sub><sup>·−</sup> 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 CO<sub>2</sub><sup>·−</sup> nucleophile, only the <i>ipso</i>-products can be obtained compared with the conventional approaches. This method offers a flexible way to convert the greenhouse gas CO<sub>2</sub> 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.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 8","pages":"3816 - 3825"},"PeriodicalIF":9.7000,"publicationDate":"2025-04-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"A general electrochemical CO2 fixation to aromatic carboxylic acids via the CO2·− intermediate using a non-transition metal electrode\",\"authors\":\"Baijing Wu, Xiaoxue Luo, Hongliang Fan, Minhua Shao, Cunpu Li, Zidong Wei\",\"doi\":\"10.1007/s11426-025-2639-8\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>CO<sub>2</sub> fixation is important for reducing the greenhouse effect and improving clean energy use. While recent studies focus on converting CO<sub>2</sub> to liquid fuels, direct fixation into high-value compounds like aromatic carboxylic acids provides an alternative path. Herein, we report a general electrochemical CO<sub>2</sub> fixation to aromatic carboxylic acids via the CO<sub>2</sub><sup>·−</sup> intermediate using a non-transition metal graphite electrode. Different from the conventional aromatic radical mechanism, in this report, CO<sub>2</sub> will gain electrons on the graphite electrode to generate CO<sub>2</sub><sup>·−</sup>, which will further attack aromatic halides to obtain the desired aromatic carboxylic acid via an aromatic nucleophilic substitution mechanism. As CO<sub>2</sub><sup>·−</sup> 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 CO<sub>2</sub><sup>·−</sup> nucleophile, only the <i>ipso</i>-products can be obtained compared with the conventional approaches. This method offers a flexible way to convert the greenhouse gas CO<sub>2</sub> 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.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>\",\"PeriodicalId\":772,\"journal\":{\"name\":\"Science China Chemistry\",\"volume\":\"68 8\",\"pages\":\"3816 - 3825\"},\"PeriodicalIF\":9.7000,\"publicationDate\":\"2025-04-28\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Science China Chemistry\",\"FirstCategoryId\":\"1\",\"ListUrlMain\":\"https://link.springer.com/article/10.1007/s11426-025-2639-8\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Science China Chemistry","FirstCategoryId":"1","ListUrlMain":"https://link.springer.com/article/10.1007/s11426-025-2639-8","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
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.
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.
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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.