The continued massive consumption of fossil fuels in modern societies has led to a range of environmental issues, including excessive CO 2 emissions. In this regard, electrochemical CO 2 reduction can convert intermittent electricity into chemical fuels and other value-added products, which holds the potential to close the carbon cycle. Among the various catalysts, metals are the most extensively studied heterogeneous CO 2 RR electrocatalysts and can be classified into three categories based on the main products. Containing Bi, Sn, In, Pb, and Cd (formate), Au, Ag, and Zn (CO), and Cu (multicarbon products).
The development of Cu-based catalysts has garnered significant attention due to the higher energy density and added value of the multicarbon products. However, the reaction network is extremely complex, involving multi-step electron/proton transfer reactions and interactions among various intermediates. Moreover, the structure of Cu catalysts undergoes dynamic reconstruction under operating conditions, which significantly affects their catalytic performance. The reconstruction process is influenced by many factors (electrolyte, electrolysis mode, catalyst structure and microenvironment, etc.). These factors constrain stability and selectivity, complicating the development of structure-activity relationships. Recent advancements in in-situ /operando characterization techniques enable real-time monitoring of the dynamic evolution. Combined with density functional theory (DFT) calculations, in-situ /operando studies can help give a picture of how catalytic sites reconstruct during electrolysis and how they influence catalytic performance.
Recently, a research team led by Prof. Chen Chen from Tsinghua University (China) presents a general overview of the recent advances regarding the dynamic surfaces of Cu-based catalysts. This review begins with the discussion of the mechanism of C 2+ product (ethylene, ethanol, acetate and propanol, etc.) generation. The structural factors promoting the generation of C 2+ products (crystal facets, low coordination sites and oxidation states) are reviewed, and the dynamic evolution of these structural factors is discussed. Subsequently, from the perspective of dynamic surfaces, the effects of cation effect and pulsed electrochemical method on the catalytic performance are discussed. Finally, it looks ahead to the further exploration of reconstruction mechanisms and the application of robotic AI chemists to study CO 2 RR. The results were published in Chinese Journal of Catalysis (https://doi.org/10.1016/S1872-2067(24)60185-3).
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About the Journal
Chinese Journal of Catalysis is co-sponsored by Dalian Institute of Chemical Physics, Chinese Academy of Sciences and Chinese Chemical Society, and it is currently published by Elsevier group. This monthly journal publishes in English timely contributions of original and rigorously reviewed manuscripts covering all areas of catalysis. The journal publishes Reviews, Accounts, Communications, Articles, Highlights, Perspectives, and Viewpoints of highly scientific values that help understanding and defining of new concepts in both fundamental issues and practical applications of catalysis. Chinese Journal of Catalysis ranks among the top one journals in Applied Chemistry with a current SCI impact factor of 15.7. The Editors-in-Chief are Profs. Can Li and Tao Zhang.
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Chinese Journal of Catalysis
Electrochemical CO2RR to C2+ products: A vision of dynamic surfaces of Cu-based catalysts
9-Jan-2025