Electrochemical reduction of CO₂ into value-added fuels and chemicals driven by renewable energy presents a potentially sustainable route to mitigate CO₂ emissions and alleviate the dependence on fossil fuels. While tailoring the electronic structure of active components to modulate their intrinsic reactivity could tune the CO₂ reduction reaction (CO₂RR), their use is limited by the linear scaling relation of intermediates. Due to the high susceptibility of the CO₂RR to the local CO₂ concentration/pH and mass transportation of CO₂/intermediates/products near the gas–solid–liquid three-phase interface, engineering catalysts’ morphological and interfacial properties holds great promise to regulate the CO₂RR, which are irrelevant with linear scaling relation and possess high resistance to harsh reaction conditions. Herein, we provide a comprehensive overview of recent advances in tuning CO₂ reduction electrocatalysis via morphology and interface engineering. The fundamentals of the CO₂RR and design principles for electrode materials are presented firstly. Then, approaches to build an efficient three-phase interface, tune the surface wettability, and design a favorable morphology are summarized; the relationship between the properties of engineered catalysts and their CO₂RR performance is highlighted to reveal the activity-determining parameters and underlying catalytic mechanisms. Finally, challenges and opportunities are proposed to suggest the future design of advanced CO₂RR electrode materials.

中文翻译：

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通过形态学和界面工程设计二氧化碳还原电极材料

用电化学方法将CO ₂还原为增值燃料和可再生能源驱动的化学物质，是缓解CO ₂排放并减轻对化石燃料依赖性的潜在可持续途径。虽然定制活性成分的电子结构以调节其固有反应性可以调节CO ₂还原反应（CO ₂ RR），但其使用受到中间体线性比例关系的限制。由于CO ₂ RR对局部CO ₂浓度/ pH和CO _2的质量转移的敏感性高/中间体/靠近气-固-液三相界面的产物，工程催化剂的形态和界面性质对调节CO ₂ RR具有广阔的前景，与线性比例关系无关，并且对苛刻的反应条件具有很高的抵抗力。在本文中，我们提供了通过形态学和界面工程调整CO ₂还原电催化的最新进展的全面概述。CO ₂的基本原理首先介绍了电极材料的RR和设计原理。然后，总结了建立有效的三相界面，调节表面润湿性和设计良好形态的方法。重点介绍了工程催化剂的性能与其CO ₂ RR性能之间的关系，以揭示活性决定参数和潜在的催化机理。最后，提出了挑战和机遇，以建议高级CO ₂ RR电极材料的未来设计。