物理化学学报 >> 2021, Vol. 37 >> Issue (5): 2006080.doi: 10.3866/PKU.WHXB202006080

所属专题: CO2还原

综述 上一篇    下一篇

基于单原子催化剂的二氧化碳选择性转化

崔新江(), 石峰()   

  • 收稿日期:2020-06-30 录用日期:2020-07-25 发布日期:2020-07-31
  • 通讯作者: 崔新江,石峰 E-mail:xinjiangcui@licp.cas.cn;fshi@licp.cas.cn
  • 作者简介:Xinjiang Cui obtained his Ph.D. degree in 2013 supervised by Prof. Youquan Deng and Prof. Feng Shi at Lanzhou Institute of Chemical Physics (LICP), Chinese Academy of Sciences. After a five- and half-year postdoctoral research in Leibniz Institute for Catalysis and École Polytechnique Fédérale de Lausanne (EPFL). Xinjiang Cui joined the faculty of LICP and is focusing on the transformation of light chain hydrocarbons and the synthesis of fine chemicals with olefins by heterogeneous catalysis
    Feng Shi completed his Ph.D. studies in catalysis at Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences (CAS) in 2004. After a three-year postdoctoral research in LIKAT in Germany, he joined the faculty of Lanzhou Institute of Chemical Physics in 2008 as Hundred Talents Program of CAS. Since 2016, Feng SHI is the deputy director of the State Key Laboratory for Oxo Synthesis and Selective Oxidation. His research focuses on nano-catalysis in fine chemical synthesis and C1 chemistry, and he has published more than 120 papers
  • 基金资助:
    国家自然科学基金(21633013);国家自然科学基金(91745106);国家自然科学基金(21925207);中国科学院西部之光和前沿科学重点研究项目(QYZDJ-SSW-SLH051)

Selective Conversion of CO2 by Single-Site Catalysts

Xinjiang Cui(), Feng Shi()   

  • Received:2020-06-30 Accepted:2020-07-25 Published:2020-07-31
  • Contact: Xinjiang Cui,Feng Shi E-mail:xinjiangcui@licp.cas.cn;fshi@licp.cas.cn
  • About author:Email: fshi@licp.cas.cn (F.S.); Tel.: +86-931-4968142 (F.S.)
    Email: xinjiangcui@licp.cas.cn (X.C.)
  • Supported by:
    the National Natural Science Foundation of China(21633013);the National Natural Science Foundation of China(91745106);the National Natural Science Foundation of China(21925207);Light of West China and Key Research Program of Frontier Sciences of CAS(QYZDJ-SSW-SLH051)

摘要:

近年来,由于其接近100%的原子利用率和独特的催化性能,单原子催化剂研究受到了极大的关注。近年来,人们针对二氧化碳选择性催化转化的单原子催化剂研究开展了大量的工作,实现了一氧化碳、甲烷、甲醇、甲酸以及C2+化合物等化学品的选择性合成。此外,通过引入胺类以及环氧化合物,二氧化碳可以催化转化为高附加值的精细化学品。本综述总结了近几年来单原子催化剂通过电催化、光催化以及热催化的方法在二氧化碳选择性还原方面的研究工作,并深入探讨单原子催化剂在二氧化碳选择还原反应中的结构性能关系以及其结构的调控对催化剂活性的影响。

关键词: CO2还原, 单原子催化, 羰基合成, 电催化, 光催化, 热催化

Abstract:

Industrial revolution has led to increased combustion of fossil fuels. Consequently, large amounts of CO2 are emitted to the atmosphere, throwing the carbon cycle out of balance. Currently, the most effective method to reduce the CO2 concentration is direct CO2 capture from the atmosphere and pumping of the captured CO2 deep underground or into the mid-ocean. The transformation of CO2 into high-value chemicals is an attractive yet challenging task. In recent years, there has been much interest in the development of CO2 utilization technologies based on electrochemical CO2 reduction, photochemical CO2 reduction, and thermal CO2 reduction, and CO2 valorization has emerged as a hot research topic. In electrochemical CO2 reduction, the cathodic reaction is the reduction of CO2 to value-added chemicals. The anodic reaction should be the oxygen evolution reaction, and water is the only renewable and scalable source of electrons and protons in this reaction. There is a plethora of research on the use of various metals to catalyze this reaction. Among these, Cu-based materials have been demonstrated to show unique catalytic activity and stability for the electrochemical conversion of CO2 to valuable fuels and chemicals. Moreover, the solar-driven conversion of CO2 into value-added chemical fuels has attracted great attention, and much effort is being devoted to develop novel catalysts for the photoreduction of CO2, especially by mimicking the natural photosynthetic process. The key step in the photocatalytic process is the efficient generation of electron-hole pairs and separation of these charge carriers. The efficient separation of photoinduced charge carriers plays a crucial role in the final catalytic activity. Compared with CO2 reduction via electrocatalysis and photocatalysis, thermal reduction is more attractive because of its potential large-scale application in the industry. Heterogeneous nanomaterials show excellent activity in the electrocatalytic, photocatalytic, and thermal catalytic conversion of CO2. However, nanostructured materials have drawbacks on the investigation of the intrinsic activity of the active sites. In recent years, single-site catalysts have become popular because they allow for maximum utilization of the metal centers, show specific catalytic performance, and facilitate easy elucidation of the catalytic mechanism at the molecular level. Accordingly, numerous single-site catalysts were developed for CO2 reduction to produce value-added chemicals such as CO, CH4, CH3OH, formate, and C2+ products. Value-added chemicals have also been synthesized with the aid of amines and epoxides. This review summarizes recent state-of-the-art single-site catalysts and their application as heterogeneous catalysts for the electroreduction, photoreduction, and thermal reduction of CO2. In the discussion, we will highlight the structure-activity relationships for the catalytic conversion of CO2 with single-site catalysts.

Key words: CO2 reduction, Single site catalyst, Carbonylation, Electrocatalysis, Photocatalysis, Thermal catalysis

MSC2000: 

  • O643