中国科学院上海高等研究院陈为团队报道，镍空心纤维上氯掺杂SnO₂纳米花在安培电流密度下增强CO₂电还原。相关研究成果于2025年1月6日发表于国际顶尖学术期刊《德国应用化学》。

可再生能源驱动的电化学二氧化碳减排，已成为未来可持续的一项有前景的技术。然而，在安培级电流密度下实现可储存液体燃料的有效生产，仍然是大规模实施二氧化碳电还原的一个重大障碍。

该文中，研究人员报告了一种新型催化电极，其包括排列在三维镍中空纤维外部的氯掺杂SnO₂纳米花。该电极在将CO₂转化为甲酸盐方面表现出卓越的电催化性能，在2 A cm^-2下实现了99%的甲酸盐选择性和93%的CO₂单程转化率。此外，它表现出优异的稳定性，在3 A cm^-2的电流密度下，甲酸盐选择性在520小时内保持在94%以上。

实验结果与理论计算相结合证实，中空纤维渗透效应促进的传质增强，再加上保留良好的Sn⁴⁺物种和Sn-Cl键，协同提高了CO₂转化的活性。将氯掺入SnO₂可以增强电子传输和CO₂吸附，大大降低关键中间体*OCHO形成的反应能量势垒，并提高甲酸盐的产量。

附：英文原文

Title: Chlorine-Doped SnO2 Nanoflowers on Nickel Hollow Fiber for Enhanced CO2 Electroreduction at Ampere-level Current Densities

Author: Yiheng Wei, Xiaotong Wang, Jianing Mao, Yanfang Song, Huanyi Zhu, Xiaohu Liu, Cheng Luo, Shoujie Li, Aohui Chen, Guihua Li, Xiao Dong, Wei Wei, Wei Chen

Issue&Volume: 2025-01-06

Abstract: Renewable energy-driven electrochemical CO2 reduction has emerged as a promising technology for a sustainable future. However, achieving efficient production of storable liquid fuels at ampere-level current densities remains a significant hurdle in the large-scale implementation of CO2 electroreduction. Here we report a novel catalytic electrode comprising chlorine-doped SnO2 nanoflowers arrayed on the exterior of three-dimensional nickel hollow fibers. This electrode demonstrates exceptional electrocatalytic performance for converting CO2 to formate, achieving a remarkable formate selectivity of 99% and a CO2 single-pass conversion rate of 93% at 2 A cm-2. Furthermore, it exhibits excellent stability, maintaining a formate selectivity of above 94% for 520 h at a current density of 3 A cm-2. Experimental results combined with theoretical calculations confirm that the enhanced mass transfer facilitated by the hollow fiber penetration effect, coupled with the well-retained Sn4+ species and Sn-Cl bonds, synergistically elevates the activity of CO2 conversion. The incorporation of chlorine into SnO2 enhances electron transport and CO2 adsorption, substantially lowering the reaction energy barrier for the crucial intermediate *OCHO formation, and boosting the formate production.

DOI: 10.1002/anie.202423370

Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202423370