Dr. Wanfeng Yang, Dr. Yong Zhao, Yiqing Chen, Hangjuan Ren, Jiameng Sun, Zhangsheng Shi, Xindie Jin, Prof. Zhonghua Zhang, Prof. Xin Wang
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引用次数: 0
Abstract
Electrocatalytic CO2 reduction (CO2R) to multi-carbon (C2+) products in strong acid presents a promising approach to mitigate the CO2 loss commonly encountered in alkaline and neutral systems. However, this process often suffers from low selectivity for C2+ products due to the competing C1 (e.g., CO and HCOOH) formation and complex C−C coupling kinetics. In this work, we report a CO2 coverage constraining strategy by diluting CO2 reactant feed to modulate the intermediate distribution and C−C coupling pathways for an enhanced electrosynthesis of C2+ products in strong acid. Lowering the CO2 feed concentration reduces CO2 coverage on copper catalyst, enriching the surface coverage and optimizing the adsorption configuration of the key CO intermediate for C−C coupling. This approach efficiently suppresses the formation of undesired C1 products. By employing a 20 % CO2 feed, we achieved a significant improvement in C2+ Faradaic efficiency, reaching 68 % at 100 mA cm−2, approximately 1.7 times higher than the 41 % obtained using pure CO2. We demonstrated the direct electroreduction of a 30 % CO2 feed—representative CO2 concentration of typical industrial flue gases—in a full electrolyzer, achieving a C2+ selectivity of 78 % and an energy efficiency of 23 % at 200 mA cm−2.
期刊介绍:
Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.