文献类型：期刊文献

中文题名：The modulating effect of N coordination on single-atom catalysts researched by Pt-N_(x)-C model through both experimental study and DFT simulation

作者：Mengmeng Fan[1,2] Jiewu Cui[2,3] Junjie Zhang[2] Jingjie Wu[4] Shuangming Chen[5] Li Song[5] Zixing Wang[2] Ao Wang[7] Robert Vajtai[2] Yucheng Wu[3] Pulickel MAjayan[2] Jianchun Jiang[7] Dongping Sun[6]

第一作者：Mengmeng Fan

机构：[1]Nanjing Forestry University,Jiangsu Co-Innovation Center for Efficient Processing and Utilization of Forest Resources,College of Chemical Engineering,Nanjing 210037,China;[2]Rice University,Department of Materials Science and NanoEngineering,Houston,TX 77005,USA;[3]Hefei University of Technology,School of Materials Science and Engineering,Hefei 230009,China;[4]University of Cincinnati,Department of Chemical and Environmental Engineering,Cincinnati,OH 45221,USA;[5]University of Science and Technology of China,National Synchrotron Radiation Laboratory,CAS Center for Excellence in Nanoscience,Hefei 230026,China;[6]Nanjing University of Science and Technology,Chemicobiology and Functional Materials Institute,Nanjing 210094,China;[7]Key Lab of Biomass Energy and Material,Jiangsu Province,Jiangsu Co-Innovation Center of Efficient Processing and Utilization of Forest Resources,Institute of Chemical Industry of Forest Products,Chinese Academy of Forestry,Nanjing 210042,China

年份：2021

期号：32

起止页码：160-167

中文期刊名：材料科学技术：英文版

外文期刊名：Journal of Materials Science & Technology

收录：CSTPCD;;Scopus;CSCD:【CSCD2021_2022】；PubMed;

基金：financially supported by the National Natural Science Foundation of China (Nos. 51572124 and 51702162);the Natural Science Foundation of Jiangsu Province (No. BK20180154and BK20180490);the Fundamental Research Funds for the Central Universities (No. 30920130111003);A Project Funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD, China)。

语种：英文

中文关键词：Modulating effect;N coordination;Single-atom catalysts;Pt-N_(x)-C model;DFT simulation

分类号：O641.4;O643.36

摘要：N-doped carbon-based single-atom catalysts(NC-SACs) are widely researched in various electrochemical reactions due to high metal atom utilization and catalytic activity.The catalytic activity of NC-SACs originates from the coordinating structure between single metal site(M) and the doped nitrogen(N) in carbon matrix by forming M-N_(x)-C structure(1≤x≤4).The M-N4-C structure is widely considered to be the most stable and effective catalytic site.However,there is no in-depth research for the "x" modulation in Pt-Nx-C structure and the corresponding catalytic properties.Herein,atomically dispersed Pt on N-doped carbon(Pt-NC) with Pt-Nx-C structure(1≤x≤4),as a research model,is fabricated by a ZIF-8 template and applied to catalytic oxygen reduction.Different carbonization temperatures are used to control N loss,and then modulate the N coordination of Pt-Nx-C structure.The Pt-NC has the predictable low half-wave potential(E_(1/2)) of 0.72 V vs RHE compared to the Pt/C 20% of 0.81 V due to low Pt content.Remarkably,the Pt-NC shows a high onset potential(1.10 V vs RHE,determined for j=-0.1 mA cm^(2)) and a high current density of 5.2 mA cm^(-2),more positive and higher than that of Pt/C 20%(0.96 V) and 4.9 mA cm^(-2),respectively.As the structural characterization and DFT simulation confirmed,the reducing PtN coordination number induces low valence of Pt atoms and low free energy of oxygen reduction,which is responsible for the improved catalytic activity.Furthermore,the Pt-NC shows high mass activity(172 times higher than that of Pt/C 20%),better stability and methanol crossover resistance.