The CO₂ electroreduction reaction (CO₂RR) is a promising approach of using renewable electricity to synthesize fuels and value-added chemicals. At present, Cu is generally considered to be the major monometallic catalyst capable of producing multicarbon products (C₂₊) with high current densities from the CO₂RR, but it still suffers from the low activity and high overpotential. The challenge of sluggish CO₂RR kinetics can be overcome by developing efficient Cu-based catalysts, which undergo the dynamic evolution during the reaction process. The dynamic evolution of the Cu-based catalysts taking place under working conditions makes it difficult to study the structure-activity correlation and reaction mechanism present during CO₂RR. Recently, a number of important works have observed and revealed the dynamic evolution process of Cu-based catalysts by operando characterization techniques. This aspect, however, remains less summarized and prospected in the CO₂RR literature. In this Review, we summarize the dynamic evolution of Cu-based catalysts during the CO₂RR from aspects of structure, composition and oxidation state. We highlight the correlations between evolution behaviors and catalytic properties. Then, we discuss the dynamic deactivation process of Cu-based catalysts during CO₂RR, including metal impurities contamination and carbon accumulation. In particular, we introduce recent advancements in in situ characterization techniques those are employed to probe the dynamic evolution under operating conditions. We end the Review by outlining the challenges and offering personal perspectives on the future development opportunities in this field.

中文翻译：

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CO2 电还原过程中铜基催化剂的动态演变


CO₂ 电还原反应 （CO₂RR） 是一种很有前途的利用可再生电力合成燃料和增值化学品的方法。目前，Cu 通常被认为是能够从 CO ₂RR 中产生具有高电流密度的多碳产物 （C₂₊） 的主要单金属催化剂，但它仍然存在低活性和高过电位的问题。通过开发高效的铜基催化剂，可以克服 CO₂RR 动力学缓慢的挑战，该催化剂在反应过程中发生动态演变。Cu 基催化剂在工作条件下发生的动态演变使得研究 CO₂ RR 过程中存在的构效相关性和反应机理变得困难。近年来，许多重要的工作通过原位表征技术观察和揭示了 Cu 基催化剂的动态演化过程。然而，这方面在 CO 2 RR 文献中仍然较少总结和展望。在本文中，我们从结构、成分和氧化态方面总结了 Cu 基催化剂在 CO 2 RR 过程中的动态演变。我们强调了进化行为和催化特性之间的相关性。然后，我们讨论了 Cu 基催化剂在 CO 2 RR 过程中的动态失活过程，包括金属杂质污染和碳积累。特别是，我们介绍了原位表征技术的最新进展，这些技术用于探测操作条件下的动态演变。 在回顾的最后，我们概述了面临的挑战，并就该领域的未来发展机会提供了个人观点。