English

Selective Conversion of CO₂ by Single-Site Catalysts

• Cui Xinjiang ^, ,
• Shi Feng ^,

• State Key Laboratory for Oxo Synthesis and Selective Oxidation, Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, Lanzhou 730000, China

Author Bio: 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;

Corresponding author: Cui Xinjiang, xinjiangcui@licp.cas.cn Shi Feng, fshi@licp.cas.cn

• Received Date: 30 June 2020
  Accepted Date: 25 July 2020
  Revised Date: 24 July 2020
  Available Online: 15 May 2021
• Fund Project:

  The project was supported by the National Natural Science Foundation of China (21633013, 91745106, 21925207), Light of West China and Key Research Program of Frontier Sciences of CAS (QYZDJ-SSW-SLH051)

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

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