Abstract
Electrochemical CO2 reduction reaction (CO2RR) is a critical route to reduce the concentration of CO2 in the atmosphere and solve the energy crisis by converting CO2 into high-value chemicals and fuels. It is therefore crucial to rationally design efficient and cost-effective electrochemical catalysts. Copper (Cu) is found to be an excellent metal catalyst that can reduce CO2 to hydrocarbons and alcohols, especially C2+ products. However, there exist some problems (such as high overpotential and poor selectivity in CO2RR) that limit the application of Cu-based catalysts. In recent years, single-atom catalysts (SACs) have become an emerging research frontier in the field of heterogeneous catalysis due to their potential high activity, selectivity, and stability. Herein, the recent progress of various Cu-based SACs for CO2RR has been reviewed, especially on the regulatory strategies for the interaction of the active site with key reaction intermediates. This interaction is important for designing the active site to optimize the multi-electron reduction step and improve the catalytic performance. Meanwhile, different design strategies, including the regulation of metal centers, Cu-based single-atom alloy catalysts (SAAs), non-metal SACs, tandem catalysts, and composite catalysts, have also been discussed. Finally, the current research challenges and future developments of SACs in CO2RR have been summarized.
摘要
电化学二氧化碳还原反应(CO2RR)通过将CO2转化为高价值化学品和燃料来降低其在大气中的浓度, 是解决能源危机的重要途径. 因此, 合理设计高效、 经济的电化学催化剂至关重要. 研究发现, 铜(Cu)是一种性能优越的金属催化剂, 可将CO2还原成碳氢化合物和醇类, 尤其是C2+产物. 然而, Cu催化剂也存在一定问题(如过电位高和CO2RR选择性差等), 从而限制了其应用. 近年来, 单原子催化剂(SACs)因其具有高活性、高选择性和高稳定性, 已成为异相催化剂领域的新兴研究前沿. 本文总结了CO2RR的各种铜基SACs的最新研究进展, 尤其是活性位点与关键反应中间产物相互作用的调控策略. 这种相互作用对于设计活性位点以及优化多电子还原步骤和提高催化性能非常重要. 同时, 本文还讨论了金属中心调控、 铜基单原子合金催化剂、非金属SACs、 串联催化剂和复合催化剂等研究前沿. 最后, 总结了SACs应用于CO2RR的挑战与展望.
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Acknowledgements
This work was financially supported by the National Natural Science Foundation of China (92061109) and the Natural Science Basic Research Program of Shaanxi (2021JCW-20 and 2022KJXX-18).
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Author contributions Yu Q supervised the project and organized the collaboration. Li X wrote the manuscript and Yu X and Yu Q revised the manuscript. All authors discussed the review, edited and commented on the manuscript.
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Xiaojiao Li is pursuing a Master degree at the School of Materials Science and Engineering, Shaanxi University of Technology, under the supervision of Prof. Qi Yu. Her research focuses on theoretical calculations of single-atom catalysts.
Qi Yu is a professor at Shaanxi Key Laboratory of Catalysis, Shaanxi University of Technology. She obtained her BSc, MSc and PhD degrees from Jilin University, followed by visiting scholar at Tsinghua University and the National University of Singapore for several years. Now she is the deputy director of Shaanxi Laboratory of Catalysis and director of Institute of Graphene at Shaanxi University of Technology. Her current research interests focus on theoretical calculations of single-atom catalysts.
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Li, X., Yu, X. & Yu, Q. Research progress on electrochemical CO2 reduction for Cu-based single-atom catalysts. Sci. China Mater. 66, 3765–3781 (2023). https://doi.org/10.1007/s40843-023-2597-8
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DOI: https://doi.org/10.1007/s40843-023-2597-8