文献类型：期刊文献

英文题名：Lewis-base ligand-reshaped interfacial hydrogen-bond network boosts CO2 electrolysis

作者：Ge, Wangxin[1,2];Tao, Haolan[3];Dong, Lei[1];Fan, Yu[1];Niu, Yanpu[3];Zhu, Yihua[2];Lian, Cheng[3];Liu, Honglai[3];Jiang, Hongliang[1];Li, Chunzhong[1,2,4]

机构：[1]East China Univ Sci & Technol, Sch Chem Engn, Key Lab Ultrafine Mat, Minist Educ, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Shanghai Engn Res Ctr Hierarch Nanomat, Sch Mat Sci & Engn, Shanghai 200237, Peoples R China;[3]East China Univ Sci & Technol, Shanghai Engn Res Ctr Hierarch Nanomat, Sch Chem & Mol Engn, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[4]Shanghai Jiao Tong Univ, Sch Chem & Chem Engn, Dept Chem Engn, Shanghai 200240, Peoples R China

年份：2024

卷号：11

期号：8

外文期刊名：NATIONAL SCIENCE REVIEW

收录：;EI(收录号：20243016762470);WOS:【SCI-EXPANDED(收录号:WOS:001272847500001)】；

基金：This work was supported by the National Key Research and Development Program (2022YFB3808400), the National Natural Science Foundation of China (22222804 and U22B20143), the Science and Technology Commission of Shanghai Municipality (22dz1205900), and the Shanghai Municipal Science and Technology Major Project.

语种：英文

外文关键词：CO2 electrolysis; electrode-electrolyte interface; Lewis acid-base interaction; hydrogen-bonding interaction; AIMD simulation

摘要：Both the catalyst and electrolyte strongly impact the performance of CO2 electrolysis. Despite substantial progress in catalysts, it remains highly challenging to tailor electrolyte compositions and understand their functions at the catalyst interface. Here, we report that the ethylenediaminetetraacetic acid (EDTA) and its analogs, featuring strong Lewis acid-base interaction with metal cations, are selected as electrolyte additives to reshape the catalyst-electrolyte interface for promoting CO2 electrolysis. Mechanistic studies reveal that EDTA molecules are dynamically assembled toward interface regions in response to bias potential due to strong Lewis acid-base interaction of EDTA(4-)-K+. As a result, the original hydrogen-bond network among interfacial H2O is disrupted, and a hydrogen-bond gap layer at the electrified interface is established. The EDTA-reshaped K+ solvation structure promotes the protonation of *CO2 to *COOH and suppressing *H2O dissociation to *H, thereby boosting the co-electrolysis of CO2 and H2O toward carbon-based products. In particular, when 5 mM of EDTA is added into the electrolytes, the Faradaic efficiency of CO on the commercial Ag nanoparticle catalyst is increased from 57.0% to 90.0% at an industry-relevant current density of 500 mA cm(-2). More importantly, the Lewis-base ligand-reshaped interface allows a range of catalysts (Ag, Zn, Pd, Bi, Sn, and Cu) to deliver substantially increased selectivity of carbon-based products in both H-type and flow-type electrolysis cells.