用于二氧化碳捕获和氢化一体化的含两性离子的酒精解决方案†。

IF 9.2 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Green Chemistry Pub Date : 2025-03-05 DOI:10.1039/d4gc05917d

Bruno A. Cândido , Marcelli L. C. Zanirati , Francisco P. dos Santos , Wilmer Villarreal , Jairton Dupont , Pedro Migowski

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引用次数: 0

摘要

研究了一种利用两性离子碱（ZBs）在酒精溶剂中捕集与转化（ICCU）的综合工艺。内盐由1,3-二甲基咪唑阳离子组成，共价连接到酚酸酯部分，与CO2反应，在醇中形成烷基碳酸酯（AKCs）。zb产率高达70%的akc并保留化学吸附的CO2，而具有相似共轭酸pKa值的叔胺只捕获少量CO2并在测试的醇中迅速释放。根据反应温度和选择的Ru催化剂，将AKCs加氢成HCOO−或甲醇。以异丙醇为溶剂，采用1,3-二甲基-2-（4-氧苯基）咪唑（ZB-p）与顺式[Ru(dppm)2Cl2]相结合的ICCU工艺，在50℃、10 bar H2条件下反应35 min，定量地将各自的AKC转化为甲酸盐。这是迄今为止报道的最活跃的ICCU系统之一，在这些温和条件下的周转频率为660 h−1。以Ru-MACHO-BH为催化剂，在140℃和70 bar H2条件下，将ZB-p的AKC在乙二醇中加氢20小时，甲醇收率为66%。

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Zwitterionic alcoholic solutions for integrated CO2 capture and hydrogenation†

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Zwitterionic alcoholic solutions for integrated CO2 capture and hydrogenation†

An integrated CO₂ capture and conversion (ICCU) process using zwitterionic bases (ZBs) in alcohol solvents was developed. Inner salts composed of a 1,3-dimethylimidazolium cation covalently attached to a phenolate moiety react with CO₂ to form alkyl carbonates (AKCs) in alcohols. The ZBs yield up to 70% AKCs and retain chemisorbed CO₂, whereas tertiary amines with similar conjugate acid pK_a values capture only small amounts of CO₂ and quickly release it in the alcohols tested. The AKCs were hydrogenated to HCOO⁻ or methanol, depending on the reaction temperature and the Ru catalyst selected. Using isopropanol as the solvent, the ICCU process combining 1,3-dimethyl-2-(4-oxyphenyl)imidazolium () and cis-[Ru(dppm)₂Cl₂] quantitatively converted the respective AKC to formate at 50 °C and 10 bar H₂ after 35 minutes of reaction. This represents one of the most active ICCU systems reported to date, with a turnover frequency of 660 h⁻¹ under these mild conditions. Methanol was obtained with a 66% yield after 20 hours by hydrogenation of the AKC of in ethylene glycol using the catalyst Ru-MACHO-BH at 140 °C and 70 bar H₂.

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来源期刊

Green Chemistry 化学-化学综合

CiteScore

16.10

自引率

7.10%

发文量

677

审稿时长

1.4 months

期刊介绍： Green Chemistry is a journal that provides a unique forum for the publication of innovative research on the development of alternative green and sustainable technologies. The scope of Green Chemistry is based on the definition proposed by Anastas and Warner (Green Chemistry: Theory and Practice, P T Anastas and J C Warner, Oxford University Press, Oxford, 1998), which defines green chemistry as the utilisation of a set of principles that reduces or eliminates the use or generation of hazardous substances in the design, manufacture and application of chemical products. Green Chemistry aims to reduce the environmental impact of the chemical enterprise by developing a technology base that is inherently non-toxic to living things and the environment. The journal welcomes submissions on all aspects of research relating to this endeavor and publishes original and significant cutting-edge research that is likely to be of wide general appeal. For a work to be published, it must present a significant advance in green chemistry, including a comparison with existing methods and a demonstration of advantages over those methods.