Oxidization-induced structural optimization of Ni_(3)Fe-N-C derived from 3D covalent organic framework for high-efficiency and durable oxygen evolution reaction  

作　　者：Haibing Meng Bin Wu Tianxiao Sun Long Wei Yunlong Zhang Bo Liu Kai Chen Zhen-Bo Wang Shuhui Sun Chunru Wang Xian-Ming Zhang 

机构地区：[1]College of Chemistry,Taiyuan University of Technology,Taiyuan 030024,China [2]Helmholtz-Zentrum Berlin für Materialien und Energie GmbH,Albert-Einstein-Straße 15,Berlin 12489,Germany [3]Institute of Physics,Humboldt University Berlin,Newton-Straße 15,Berlin 12489,Germany [4]National Synchrotron Radiation Laboratory,University of Science and Technology of China,Hefei 230026,China [5]MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage,School of Chemistry and Chemical Engineering,Harbin Institute of Technology,Harbin 150001,China [6]Institute National de La Recherche Scientifique(INRS)-CentreÉnergie Matériaux Télécommunications,Varennes,QC J3X 1P7,Canada [7]Beijing National Laboratory for Molecular Sciences,CAS Key Laboratory of Molecular Nanostructure and Nanotechnology,Institute of Chemistry,Chinese Academy of Sciences,Beijing 100190,China

出　　处：《Nano Research》2023年第5期6710-6720,共11页纳米研究（英文版）

基　　金：the National Natural Science Foundation of China(Nos.22075062 and 21871167)and the Volkswagen Foundation(Freigeist Fellowship)。

摘　　要：NiFe composites have been regarded as promising candidates to replace commercial noble-based electrocatalysts for the oxygen evolution reaction(OER).However,their practical applications still suffer from poor conductivity,limited activity,durability.To address these issues,herein,by utilizing three-dimensional covalent organic framework(3D-COF)with porous confined structures and abundant coordinate N sites as the precursor,the partially oxidized Ni_(3)Fe nanoalloys wrapped by Ndoped carbon(N-C)layers are constructed via simple pyrolysis and subsequent oxidization.Benefiting from the 3D curved hierarchical structure,high-conductivity of Ni_(3)Fe and N-C layers,well-distributed active sites,the as-synthesized O-Ni_(3)Fe-NC catalyst demonstrates excellent activity and durability for catalyzing OER.Experimental and theoretical analyses disclose that both high-temperature oxidization and the OER process greatly promote the formation and exposure of the Ni(Fe)OOH active species as well as lower charge transfer resistance,inducing its optimized OER activity.The robust graphitized N-C layers with superior conductivity and their couplings with oxidized Ni_(3)Fe nanoalloys are beneficial for stabilizing catalytic centers,thereby imparting O-Ni_(3)Fe-N-C with such outstanding stability.This work not only provides a rational guidance for enriching and stabilizing high-activity catalytic sites towards OER but also offers more insights into the structural evolution of NiFe-based OER catalysts.

关 键 词：three-dimensional covalent organic framework(3D-COF) Ni_(3)Fe graphitized N-C layer structure optimization durability 

分 类 号：TM911.4[电气工程—电力电子与电力传动] O643.36[理学—物理化学]