Steering CO_(2)electrolysis selectivity by modulating the local reaction environment:An online DEMS approach for Cu electrodes  

作　　者：Ke Ye Guiru Zhang Baoxin Ni Liang Guo Chengwei Deng Xiaodong Zhuang Changying Zhao Wen-Bin Cai Kun Jiang 

机构地区：[1]Interdisciplinary Research Center,School of Mechanical Engineering,Shanghai Jiao Tong University,Shanghai 200240,China [2]China-UK Low Carbon College,Shanghai Jiao Tong University,Shanghai 201306,China [3]State Key Laboratory of Space Power-Sources Technology,Shanghai Institute of Space Power Sources,Shanghai 200245,China [4]School of Chemistry and Chemical Engineering,Frontiers Science Center for Transformative Molecules,Shanghai Jiao Tong University,Shanghai 200240,China [5]Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials,Collaborative Innovation Center of Chemistry for Energy Materials,Department of Chemistry,Fudan University,Shanghai 200438,China

出　　处：《eScience》2023年第4期89-98,共10页电化学与能源科学（英文）

基　　金：supported by the National Key R&D Program of China(2022YFB4102000,2022YFA1505100,2022YFA1503803);the NSFC(22002088);the Shanghai Sailing Program(20YF1420500);the Shanghai Science and Technology Innovation Action Plan(22dz1205500).

摘　　要：Electrochemical CO_(2)reduction is a typical surface-mediated reaction,with its reaction kinetics and product distributions largely dependent on the dynamic evolution of reactive species at the cathode–catholyte interface and on the resultant mass transport within the hydrodynamic boundary layer in the vicinity of the cathode.To resolve the complex local reaction environment of branching CO_(2)reduction pathways,we here present a dif-ferential electrochemical mass spectroscopic(DEMS)approach for Cu electrodes to investigate CO_(2)mass trans-port,the local concentration gradients of buffering anions,and the Cu surface topology effects on CO_(2)electrolysis selectivity at a temporal resolution of~400 ms.As a proof of concept,these tuning knobs were validated on an anion exchange membrane electrolyzer,which delivered a Faradaic efficiency of up to 40.4%and a partial current density of 121 mA cm^(-2)for CO_(2)-to-C_(2)H_(4)valorization.This methodology,which bridges the study of fundamental surface electrochemistry and the upgrading of practical electrolyzer performance,could be of general interest in helping to achieve a sustainable circular carbon economy.

关 键 词：SPECTROELECTROCHEMISTRY CO_(2)reduction reaction Copper electrode Differential electrochemical mass spectroscopy Local reaction environment 

分 类 号：O64[理学—物理化学]