物理化学学报 >> 2021, Vol. 37 >> Issue (5): 2010022.doi: 10.3866/PKU.WHXB202010022

所属专题: CO2还原

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离子液体介导CO2化学转化研究进展

王欢1,2, 吴云雁1,2, 赵燕飞1,2, 刘志敏1,2,3,*()   

  1. 1 中国科学院化学研究所,北京分子科学国家实验室,胶体与界面与热力学重点实验室,中国科学院化学研究所分子科学卓越教育中心,北京 100190
    2 中国科学院大学,北京 100049
    3 北京市怀柔国家综合科学中心物理科学实验室,北京 101400
  • 收稿日期:2020-10-12 录用日期:2020-10-30 发布日期:2020-11-04
  • 通讯作者: 刘志敏 E-mail:liuzm@iccas.ac.cn
  • 作者简介:刘志敏,1968年生。1997年在中国石油大学(北京)获博士学位;1997年9月至1999年8月在中国科学院化学研究所做博士后研究。现任中国科学院化学研究所研究员。主要研究方向集中于绿色溶剂与可再生碳资源转化利用方面
  • 基金资助:
    国家自然科学基金(21890761);国家自然科学基金(21533011);北京市物质科学中心(Z191100007219009)

Recent Progress on Ionic Liquid-Mediated CO2 Conversion

Huan Wang1,2, Yunyan Wu1,2, Yanfei Zhao1,2, Zhimin Liu1,2,3,*()   

  1. 1 Beijing National Laboratory for Molecular Sciences, Key Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Center for Excellence in Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China
    2 University of Chinese Academy of Sciences, Beijing 100049, China
    3 Physical Science Laboratory, Huairou National Comprehensive Science Center, Beijing 101400, China
  • Received:2020-10-12 Accepted:2020-10-30 Published:2020-11-04
  • Contact: Zhimin Liu E-mail:liuzm@iccas.ac.cn
  • About author:Zhimin Liu. Email: liuzm@iccas.ac.cn. Tel.: +86-10-62562852
  • Supported by:
    National Natural Science Foundation of China(21890761);National Natural Science Foundation of China(21533011);Beijing Municipal Science & Technology Commission, China(Z191100007219009)

摘要:

高效利用CO2资源对绿色可持续发展具有重要意义。近年来,高效催化转化CO2为高附加值化学品的研究广受关注。但是,由于CO2高的热力学稳定性和动力学惰性,其化学转化往往需要高反应活性的底物和苛刻的反应条件。因此,科研工作者致力于发展催化转化CO2的高性能催化剂和新方法。迄今,已经发展了一系列多相和均相催化剂用于催化转化CO2。在众多性能优异的催化剂中,离子液体因其独特的性能,可实现温和甚至室温条件下高效转化CO2为高附加值化学品,而被广泛研究。具有特定官能团的功能化离子液体可以作为溶剂、CO2吸附剂、CO2活化剂以及催化剂或共催化剂,实现无金属条件下高效催化转化CO2;各种金属-离子液体耦合催化体系可实现协同催化转化CO2为高附加值化学品。在本文中,我们总结了近期离子液体介导的、通过构筑C—O、C—N、C—S、C—H以及C—C键,转化CO2合成化学品的研究。主要概述了近年来离子液体在化学吸附活化CO2、催化转化CO2制备碳酸酯和含N/S杂原子的化合物以及催化CO2加氢制备甲酸、乙酸、甲烷、低碳产物等方面的研究进展,并对相关反应路径和机理进行了探讨。在离子液体催化反应体系中,离子液体不仅可以活化CO2还可以通过氢键作用活化底物,从而协同催化CO2的转化。在本文的最后,对相关研究的不足及未来发展前景进行了探讨和展望。总之,离子液体介导的高效催化转化CO2方法为制备高价值化学品提供了绿色合成路线,具有广阔的应用前景。

关键词: CO2, 离子液体, 转化, 催化, 高附加值化学品

Abstract:

The efficient utilization of carbon dioxide (CO2) as a C1 feedstock is of great significance for green and sustainable development. Therefore, the efficient chemical conversion of CO2 into value-added products has recently attracted a lot of research attention in recent years. The transformation of CO2 generally requires high-energy substrates, specific catalysts, and harsh reaction conditions due to its high thermodynamic stability and kinetic inertness. Consequently, several efforts have been dedicated toward the development of high-performance catalysts and new reaction routes for CO2 conversion over the last few decades. To date, many routes of convert CO2 into value-added chemicals have been proposed, together with the development of heterogeneous and homogeneous catalysts. Among the advanced catalysts reported to date, ionic liquids (ILs) have been widely investigated and show great potential for the efficient, selective, and economical conversion of CO2 into highly valuable products under mild conditions, even under ambient conditions. Some task-specific ILs have been designed with unique functional groups (e.g., —OH, —SO3H, —NH2, —COOH, and —C≡N), which can act as the solvent, absorbent, activating agent, catalyst, or cocatalyst to realize the transformation of CO2 under metal-free and mild conditions. In addition, a variety of catalytic systems composed of ILs and metal catalysts have also been reported for the transformation of CO2, in which the combination of the IL and metal catalyst is responsible for CO2 conversion with high efficiency. In this review article, we summarize the recent advances in IL-mediated CO2 transformation into chemicals prepared via C—O, C—N, C—S, C—H, and C—C bond forming processes. ILs that can chemically capture CO2 with high capacity are first introduced, which can activate CO2 via the formation of IL-based carbonates or carbamates, thus realizing the transformation of CO2 under metal-free and mild conditions. Recent progress in IL-mediated CO2 transformations to form carbonates and various kinds of N- and S-containing compounds (e.g., oxazolidinones, ureas, benzimidazolones, formamides, methylamines, benzothiazoles, and other chemicals) as well as CO2 hydrogenation to give formic acid, methane, acetic acid, low-carbon alcohols, and hydrocarbons has been summarized in this review with a focus on the reaction routes, catalytic systems, and reaction mechanism. In these reactions, ILs can simultaneously activate the substrate via strong H-bonding in addition to activating CO2, and the cooperative effects among the ionic and molecular species and metal catalysts accomplish the reactions of CO2 with various kinds of substrates to afford a wide range of value-added chemicals. Finally, the shortcomings and perspectives of ILs are discussed. In short, IL-mediated CO2 transformations provide green and effective routes for the synthesis of high-value chemicals, which may have great potential for a wide range of applications.

Key words: CO2, Ionic liquid, Conversion, Catalysis, Value-added chemicals

MSC2000: 

  • O643