Tang Yu-Feng, Liu Lin-Bo, Yu Mulin, Liu Shuo, Sui Peng-Fei, Sun Wei, Fu Xian-Zhu, Luo Jing-Li, Liu Subiao
School of Minerals Processing and Bioengineering, Central South University, Changsha, Hunan 410083, China.
Department of Chemical and Materials Engineering, University of Alberta, Edmonton, Alberta T6G 1H9, Canada.
Chem Soc Rev. 2024 Sep 16;53(18):9344-9377. doi: 10.1039/d4cs00229f.
Electrochemical CO reduction (ECR) holds great potential to alleviate the greenhouse effect and our dependence on fossil fuels by integrating renewable energy for the electrosynthesis of high-value fuels from CO. However, the high thermodynamic energy barrier, sluggish reaction kinetics, inadequate CO conversion rate, poor selectivity for the target product, and rapid electrocatalyst degradation severely limit its further industrial-scale application. Although numerous strategies have been proposed to enhance ECR performances from various perspectives, scattered studies fail to comprehensively elucidate the underlying effect-performance relationships toward ECR. Thus, this review presents a comparative summary and a deep discussion with respect to the effects strongly-correlated with ECR, including intrinsic effects of materials caused by various sizes, shapes, compositions, defects, interfaces, and ligands; structure-induced effects derived from diverse confinements, strains, and fields; electrolyte effects introduced by different solutes, solvents, cations, and anions; and environment effects induced by distinct ionomers, pressures, temperatures, gas impurities, and flow rates, with an emphasis on elaborating how these effects shape ECR electrocatalytic activities and selectivity and the underlying mechanisms. In addition, the challenges and prospects behind different effects resulting from various factors are suggested to inspire more attention towards high-throughput theoretical calculations and / techniques to unlock the essence of enhanced ECR performance and realize its ultimate application.
电化学CO还原（ECR）通过整合可再生能源将CO电合成高价值燃料，在缓解温室效应以及减少我们对化石燃料的依赖方面具有巨大潜力。然而，高的热力学能垒、缓慢的反应动力学、不足的CO转化率、对目标产物的选择性差以及电催化剂的快速降解严重限制了其进一步的工业规模应用。尽管已经从各个角度提出了许多提高ECR性能的策略，但分散的研究未能全面阐明与ECR相关的潜在效应-性能关系。因此，本综述对与ECR密切相关的效应进行了比较总结和深入讨论，包括由各种尺寸、形状、组成、缺陷、界面和配体引起的材料固有效应；由不同的限制、应变和场产生的结构诱导效应；由不同的溶质、溶剂、阳离子和阴离子引入的电解质效应；以及由不同的离聚物、压力、温度、气体杂质和流速引起的环境效应，重点阐述了这些效应如何塑造ECR电催化活性和选择性以及潜在机制。此外，还提出了各种因素导致的不同效应背后的挑战和前景，以激发对高通量理论计算和/技术的更多关注，从而揭示增强ECR性能的本质并实现其最终应用。
