Asymmetric electrode design with built-in nitrogen transfer channel achieving maximized three-phase reaction region for electrochemical ammonia synthesis

作     者：Chao Wang Qiyang Cheng Mengfan Wang Sisi Liu Yanzheng He Chengwei Deng Yi Sun Tao Qian Na Xu Federico Rosei Chenglin Yan 

作者机构：Collaborative Innovation Center of Suzhou Nano Science and TechnologyCollege of EnergySoochow UniversitySuzhouChina Aerospace Hydrogen Energy Technology(Shanghai)Co.Ltd.ShanghaiChina School of Chemistry and Chemical EngineeringNantong UniversityNantongChina Light Industry Institute of Electrochemical Power SourcesSuzhouChina Institut National de la Recherche ScientifiqueVarennesQuebecCanada 

出 版 物：《Electron》 (电子（英文）)

年 卷 期：2023年第1卷第1期

页      面：50-58页

学科分类：081704[工学-应用化学] 07[理学] 070304[理学-物理化学(含∶化学物理)] 08[工学] 0817[工学-化学工程与技术] 0703[理学-化学] 

基　　金：National Natural Science Foundation of China,Grant/Award Numbers:U21A20332,52103226,52202275,52203314,12204253 Distinguished Young Scholars Fund of Jiangsu Province,Grant/Award Number:BK20220061 Fellowship of China Postdoctoral Science Foundation,Grant/Award Number:2021M702382 Suzhou Foreign Academician Workstation,Grant/Award Number:SWY2022001 

主　　题：ammonia synthesis asymmetric electrode nitrogen reduction nitrogen transfer threephase reaction region 

摘      要：Carbon-free electrochemical nitrogen reduction reaction(NRR)is an appealing strategy for green ammonia synthesis,but there is still a significant performance *** working electrode is usually flooded by the electrolyte during the NRR test,and only the surface material could get access to the nitrogen,which inevitably gives rise to sluggish reaction ***,an asymmetric electrode design is proposed to tackle this *** aerophilic layer is constructed on one face of the electrocatalyst-loaded electrode,while the other side maintains its original structure,aiming to achieve facilitated nitrogen transfer and electrolyte permeation within the conductive skeleton *** asymmetric architecture affords extensive threephase reaction region within the electrode as demonstrated by the combination of theoretical simulations and experimental measurements,which gives full play to the loaded *** expected,the proofof-concept asymmetric electrode delivers an NH_(3)yield rate of 40.81μg h^(−1)mg^(−1)and a Faradaic efficiency of 71.71%at−0.3 V versus the reversible hydrogen electrode,which are more than 4 and 7 times that of conventional electrode,*** work presents a versatile strategy for enhancing the interfacial reaction kinetics and is instructive to electrode design for gas-involved electrochemical reactions.