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电化学CO还原中的稳定性问题:基础认识与设计策略的最新进展

Stability Issues in Electrochemical CO Reduction: Recent Advances in Fundamental Understanding and Design Strategies.

作者信息

Lai Wenchuan, Qiao Yan, Wang Yanan, Huang Hongwen

机构信息

College of Materials Science and Engineering, Hunan University, Changsha, Hunan, 410082, P. R. China.

College of Chemistry and Materials Science, Nanjing Normal University, Nanjing, Jiangsu, 210023, P. R. China.

出版信息

Adv Mater. 2023 Dec;35(51):e2306288. doi: 10.1002/adma.202306288. Epub 2023 Oct 30.

Abstract

Electrochemical CO reduction reaction (CO RR) offers a promising approach to close the anthropogenic carbon cycle and store intermittent renewable energy in fuels or chemicals. On the path to commercializing this technology, achieving the long-term operation stability is a central requirement but still confronts challenges. This motivates to organize the present review to systematically discuss the stability issue of CO RR. This review starts from the fundamental understanding on the destabilization mechanisms of CO RR, with focus on the degradation of electrocatalyst and change of reaction microenvironment during continuous electrolysis. Subsequently, recent efforts on catalyst design to stabilize the active sites are summarized, where increasing atomic binding strength to resist surface reconstruction is highlighted. Next, the optimization of electrolysis system to enhance the operation stability by maintaining reaction microenvironment especially mitigating flooding and carbonate problems is demonstrated. The manipulation on operation conditions also enables to prolong CO RR lifespan through recovering catalytically active sites and mass transport process. This review finally ends up by indicating the challenges and future opportunities.

摘要

电化学一氧化碳还原反应(CO RR)为闭合人为碳循环以及将间歇性可再生能源存储于燃料或化学品中提供了一种很有前景的方法。在该技术商业化的道路上,实现长期运行稳定性是一项核心要求,但仍面临挑战。这促使我们组织本次综述,系统地讨论CO RR的稳定性问题。本综述从对CO RR失稳机制的基本理解入手,重点关注连续电解过程中电催化剂的降解和反应微环境的变化。随后,总结了近期在催化剂设计方面为稳定活性位点所做的努力,其中强调了提高原子结合强度以抵抗表面重构。接下来,展示了通过维持反应微环境,特别是缓解水淹和碳酸盐问题来优化电解系统以提高运行稳定性。对操作条件的调控还能够通过恢复催化活性位点和传质过程来延长CO RR的寿命。本综述最后指出了挑战和未来机遇。

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