文献类型：期刊文献

英文题名：Modulating Interfacial Hydrogen-Bond Environment by Electrolyte Engineering Promotes Acidic CO2 Electrolysis

作者：Ge, Wangxin[1,2];Dong, Lei[1];Wang, Chaochen[2];Zhu, Yihua[2];Liu, Zhen[1];Jiang, Hongliang[1];Li, Chunzhong[1,2,3]

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]Shanghai Jiao Tong Univ, Sch Chem & Chem Engn, Dept Chem Engn, Shanghai 200240, Peoples R China

年份：2024

卷号：14

期号：14

起止页码：10529

外文期刊名：ACS CATALYSIS

收录：;EI(收录号：20242716605204);WOS:【SCI-EXPANDED(收录号:WOS:001258186700001)】；

基金：This work was supported by the National Natural Science Foundation of China (22222804 and U22B20143), the National Key R&D program (2022YFB3808400), 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：acidic CO2 electroreduction; electrode-electrolyteinterface; hydrogen-bond chemistry; electrolyteengineering; in situ spectroscopy

摘要：Acidic CO2 electroreduction offers a promising strategy for achieving a high CO2 utilization efficiency. However, it is highly challenging to inhibit the competing hydrogen evolution reactions (HER) due to the high concentration of protons at the electrode-electrolyte interface. The interfacial hydrogen-bond environment greatly affects proton transfer and the kinetics of hydrogen-related reactions, e.g., HER and CO2 reduction. In this work, we demonstrate that sulfonate-based electrolyte additives, including sodium p-styrenesulfonate (SPS), sodium p-toluene sulfonate (STS), and sodium benzenesulfonate (SBS), enable reconstruction of the interfacial hydrogen-bond environment and enhance the CO2 electrolysis performance. Mechanistic studies uncover that the strong hydrogen-bond interactions of these sulfonate-based additives with H2O achieve the construction of a low proton-flux interface. This leads to the suppression of proton concentration-dependent HER. The SPS-assisted acidic CO2 electrolysis yields CO with a high selectivity of 97.8% and a high single-pass carbon efficiency of 66.3% at 250 mA cm(-2) on commercial Ag catalysts in acid. This work provides a facile strategy to promote acidic CO2 electrolysis by modulating the interfacial hydrogen-bond environment through electrolyte design.