Constraining CO2 Coverage on Copper Promotes CO2 Electroreduction to Multi-carbon Products in Strong Acid

IF 16.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
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.

Abstract Image

限制铜上的CO2覆盖促进强酸条件下CO2电还原生成多碳产物
在强酸中,电催化CO2还原(CO2R)为多碳(C2+)产物提供了一种很有前途的方法,可以减轻碱性和中性体系中常见的CO2损失。然而,由于竞争性的C1(如CO和HCOOH)形成和络合物C - C耦合动力学,该过程通常存在C2+产物选择性低的问题。在这项工作中,我们报告了一种CO2覆盖限制策略,通过稀释CO2反应物进料来调节中间分布和C - C偶联途径,以增强强酸中C2+产物的电合成。降低CO2进料浓度可降低铜催化剂上的CO2覆盖率,增加铜催化剂的表面覆盖率,优化C - C偶联过程中关键CO中间体的吸附构型。这种方法有效地抑制了不需要的C1产物的形成。通过使用20%的CO2进料,我们实现了C2+法拉第效率的显著提高,在100 mA cm‐2时达到68%,比使用纯CO2获得的41%高出约1.7倍。我们演示了在全电解槽中直接电还原30%的CO2进料(典型工业烟气的CO2浓度代表),在200 mA cm‐2下实现了78%的C2+选择性和23%的能源效率。
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来源期刊
CiteScore
26.60
自引率
6.60%
发文量
3549
审稿时长
1.5 months
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.
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