Broadly,the oxygen evolution reaction(OER)has been deeply understood as a significant part of energy conversion and storage.Nevertheless,the anions in the OER catalysts have been neglected for various reasons such as ...Broadly,the oxygen evolution reaction(OER)has been deeply understood as a significant part of energy conversion and storage.Nevertheless,the anions in the OER catalysts have been neglected for various reasons such as inactive sites,dissolution,and oxidation,amongst others.Herein,we applied a model catalyst s-Ni(OH)2 to track the anionic behavior in the catalyst during the electrochemical process to fill this gap.The advanced operando synchrotron radiation Fourier transform infrared(SR-FTIR)spectroscopy,synchrotron radiation photoelectron spectroscopy(SRPES)depth detection and differential X-ray absorption fine structure(D-XAFS)spectrum jointly point out that some oxidized sulfur species(SO_(4)^(2-))will selfoptimize new Ni–S bonds during OER process.Such amazing anionic self-optimization(ASO)behavior has never been observed in the OER process.Subsequently,the optimization-derived component shows a significantly improved electrocatalytic performance(activity,stability,etc.)compared to reference catalyst Ni(OH)_(2).Theoretical calculation further suggests that the ASO process indeed derives a thermodynamically stable structure of the OER catalyst,and then gives its superb catalytic performance by optimizing the thermodynamic and kinetic processes in the OER,respectively.This work demonstrates the vital role of anions in the electrochemical process,which will open up new perspectives for understanding OER and provide some new ideas in related fields(especially catalysis and chemistry).展开更多
基金supported in part by the National Key R&D Program of China(2017YFA0303500)the National Natural Science Foundation of China(U1932201,21727801,and 51902303)+4 种基金the National Natural Science Foundation of China-Ministry of Foreign Affairs and International Cooperation of Italy(51861135202)CAS International Partnership Program(211134KYSB20190063)Key Research Program of Frontier Sciences(QYZDB-SSW-SLH018)the University of Science and Technology of China start-up fundCAS Interdisciplinary Innovation Team。
文摘Broadly,the oxygen evolution reaction(OER)has been deeply understood as a significant part of energy conversion and storage.Nevertheless,the anions in the OER catalysts have been neglected for various reasons such as inactive sites,dissolution,and oxidation,amongst others.Herein,we applied a model catalyst s-Ni(OH)2 to track the anionic behavior in the catalyst during the electrochemical process to fill this gap.The advanced operando synchrotron radiation Fourier transform infrared(SR-FTIR)spectroscopy,synchrotron radiation photoelectron spectroscopy(SRPES)depth detection and differential X-ray absorption fine structure(D-XAFS)spectrum jointly point out that some oxidized sulfur species(SO_(4)^(2-))will selfoptimize new Ni–S bonds during OER process.Such amazing anionic self-optimization(ASO)behavior has never been observed in the OER process.Subsequently,the optimization-derived component shows a significantly improved electrocatalytic performance(activity,stability,etc.)compared to reference catalyst Ni(OH)_(2).Theoretical calculation further suggests that the ASO process indeed derives a thermodynamically stable structure of the OER catalyst,and then gives its superb catalytic performance by optimizing the thermodynamic and kinetic processes in the OER,respectively.This work demonstrates the vital role of anions in the electrochemical process,which will open up new perspectives for understanding OER and provide some new ideas in related fields(especially catalysis and chemistry).
