文献类型：期刊文献

英文题名：Dynamically Formed Surfactant Assembly at the Electrified Electrode-Electrolyte Interface Boosting CO2 Electroreduction

作者：Ge, Wangxin[1,2];Chen, Yuxin[3];Fan, Yu[1];Zhu, Yihua[1,2];Liu, Honglai[3];Song, Li[4];Liu, Zhen[1];Lian, Cheng[3];Jiang, Hongliang[1];Li, Chunzhong[1,2]

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 Engn, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[4]Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Hefei 230029, Anhui, Peoples R China

年份：2022

卷号：144

期号：14

起止页码：6613

外文期刊名：JOURNAL OF THE AMERICAN CHEMICAL SOCIETY

收录：;EI(收录号：20221612006579);WOS:【SCI-EXPANDED(收录号:WOS:000790698300052)】；

基金：This work was supported by the National Natural Science Foundation of China (21838003, 91834301, 21978278, and 21978087), the Shanghai Scientific and Technological Innovation Project (18JC1410500 and 19JC1410400), and the Fundamental Research Funds for the Central Universities (222201718002). The authors thank the Shanghai synchrotron Radiation Facility (14W1, SSRF), the Beijing Synchrotron Radiation Facility (1W1B and soft-X-ray endstation, BSRF), and the Hefei Synchrotron Radiation Facility (photoemission, magnetic circular dichroism and catalysis/surface science endstations, and endstations at National Synchrotron Radiation Laboratory).

语种：英文

外文关键词：Molecular dynamics - Electrochemical electrodes - Additives - Dyes - Electrolytes - Electrolytic reduction - Electrocatalysis - Cationic surfactants - Reaction kinetics - Carbon dioxide

摘要：Electrocatalytic reactions occur in the nanoscalespace at the electrified electrode-electrolyte interface. It is wellknown that the electrode-electrolyte interface, also called asinterfacial microenvironment, is difficult to investigate due to theinterference of bulk electrolytes and its dynamic evolution inresponse to applied bias potential. Here, we employ electro-chemical co-reduction of CO2and H2O on commercial Agelectrodes as a model system, in conjunction with quaternaryammonium cationic surfactants as electrolyte additives. We probebias-potential-driven dynamic response of the interfacial micro-environment as well as the mechanistic origin of catalyticselectivity. By virtue of comprehensive in situ vibrationalspectroscopy, electrochemical impedance spectroscopy, andmolecular dynamics simulations, it is revealed that the structure of surfactants is dynamically changed from a random distributionto a nearly ordered assembly with increasing bias potential. The nearly ordered surfactant assembly regulates the interfacial waterenvironment by repelling isolated water and suppressing water orientation into an ordered structure as well as promotes CO2enrichment at the electrified interface. Eventually, the formed hydrophobic-aerophilic interface microenvironment reduces theactivity of water dissociation and increases the selectivity of CO2electroreduction to CO. These results highlight the importance ofregulating the interfacial microenvironment by organic additives as a means of boosting the electrochemical performance inelectrosynthesis and beyond