Citation: Zhang Xuehua, Cao Yanwei, Chen Qiongyao, Shen Chaoren, He Lin. Recent Progress in Homogeneous Reductive Carbonylation of Carbon Dioxide with Hydrogen[J]. Acta Physico-Chimica Sinica, ;2021, 37(5): 200705. doi: 10.3866/PKU.WHXB202007052 shu

Recent Progress in Homogeneous Reductive Carbonylation of Carbon Dioxide with Hydrogen

Zhang Xuehua ^1,2 ,
Cao Yanwei ² ,
Chen Qiongyao ² ,
Shen Chaoren ² ,
He Lin ^2,3,,

1.
School of Chemistry and Environmental Engineering, Yancheng Teachers University, Yancheng 224007, Jiangsu Province, China
2.
State Key Laboratory for Oxo Synthesis and Selective Oxidation, Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, Lanzhou 730000, China
3.
Dalian National Laboratory for Clean Energy, CAS, Dalian 116023, Liaoning Province, China

Corresponding author: He Lin, helin@licp.cas.cn
Received Date: 20 July 2020
Revised Date: 3 August 2020
Accepted Date: 3 August 2020
Available Online: 6 August 2020
Fund Project: Foundation research project of Jiangsu Province, China BK20180249the Dalian National Laboratory For Clean Energy (DNL) Cooperation Fund, the CAS DNL 201919the National Natural Science Foundation of China 21802151the Natural Science Foundation of the Jiangsu Higher Education Institutions of China 18KJB150033The project was supported by the National Natural Science Foundation of China (21802151), Foundation research project of Jiangsu Province, China (BK20180249), the Dalian National Laboratory For Clean Energy (DNL) Cooperation Fund, the CAS (DNL 201919) and the Natural Science Foundation of the Jiangsu Higher Education Institutions of China (18KJB150033)

The efficient utilization of the greenhouse gas CO₂ as a C1 feedstock can effectively reduce its emission and create economic value. Hence, the efficient chemical conversion of CO₂ has been receiving intense attention. Due to the extremely low energy level of the CO₂ molecule, the high energy barrier is the primary challenge for the chemical conversion of CO₂. The chemical conversion of CO₂ is mainly carried out through non-reductive transformation in industrial. Yet, the new route of chemical synthesis based on CO₂ reductive transformation is an interesting topic to expand its resource utilization. In this context, homogeneous reductive carbonylation is a hot topic for the utilization of CO₂ via reductive transformation. In this process, the metal hydride intermediate derived from the activation of the hydrogen source is crucial to the CO₂ reduction. Hydrogen, a clean source with high atom economy, can be used as a reducing agent for the reductive conversion of inert CO₂ through carbonylation, to construct C―O, C―N, and C―C bonds and to synthesize aldehyde/alcohol, carboxylic acid, ester, amide, and other chemicals. These expand the scope of CO₂ high-value utilization and show great potential application in terms of resource utilization and environmental protection. This CO₂ utilization process is thought to involve cascading catalytic reactions of CO₂ reduction and carbonylation. The catalytic systems require the corresponding catalysts to efficiently promote each step and effectively inhibit undesired side reactions. Recently, considerable progress has been made in the homogeneous reductive carbonylation of CO₂ with H₂. However, this kind of reaction is mostly of the cascade type, and hence, requires harsh conditions and noble metal catalysts. The chemoselectivity is low because of the multiple competing reactions. In addition, due to the steric hindrance and electronic effects of the substrate, there are limitations on the types of substrates that can be employed. With the development of new characterization techniques and theoretical calculations, some progress has been made in revealing the reaction mechanism and in the activation of the carbon-oxygen bonds of CO₂. Therefore, there is an urgent need to develop a more efficient catalytic system that requires mild conditions for reductive carbonylation. In this review, we provide an overview of the groundbreaking studies and the recent breakthroughs that have demonstrated the potential of metal catalysts to utilize the combination of CO₂ and H₂ as a C1 synthon, including olefin carbonylation, amine carbonylation, and alcohol/ether carbonylation, while highlighting the effect of different types of metal catalysts on the reaction. We conclude with a perspective on the future prospects of the homogeneous reductive carbonylation of CO₂ with H₂, providing readers a snapshot of this rapidly evolving field.
- Carbon dioxide,
- Hydrogen,
- Reduction,
- Homogeneous catalysis,
- Carbonylation
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沈阳化工大学材料科学与工程学院沈阳 110142