Atomic manganese coordinated to nitrogen and sulfur for oxygen evolution  

作　　者：Xue Bai Liming Wang Bing Nan Tianmi Tang Xiaodi Niu Jingqi Guan 

机构地区：[1]Institute of Physical Chemistry,College of Chemistry,Jilin University,2519 Jiefang Road,Changchun 130021,China [2]College of Food Science and Engineering,Jilin University,Changchun 130062,China [3]CAS Key Laboratory for Biomedical Effects of Nanomaterials and Nanosafety&CAS-HKU Joint Laboratory of Metallomics on Health and Environment,Institute of High Energy Physics,Chinese Academy of Sciences,Beijing 100049,China [4]State Key Laboratory of Natural and Biomimetic Drugs,School of Pharmaceutical Sciences,Peking University,Beijing 100191,China [5]Shanghai Synchrotron Radiation Facility,Shanghai Advanced Research Institute,Chinese Academy of Science,Shanghai 201210,China

出　　处：《Nano Research》2022年第7期6019-6025,共7页纳米研究（英文版）

基　　金：supported by the National Natural Science Foundation of China(Nos.22075099 and 31971322);the Education Department of Jilin Province(JJKH20220967KJ);the National Basic Research Program of China(Nos.2016YFA0203200 and 2020YFA0710702);CAS President’s International Fellowship Initiative(PIFI,2021PM0059);the State Key Laboratory of Natural and Biomimetic Drugs,Peking University.

摘　　要：Lack of high-efficiency,cost-efficient,and well-stocked oxygen evolution reaction(OER)electrocatalysts is a main challenge in large-scale implementation of electrolytic water.By regulating the electronic structure of isolated single-atom metal sites,highperformance transition-metal-based catalysts can be fabricated to greatly improve the OER performance.Herein,we demonstrate single-atom manganese coordinated to nitrogen and sulfur species in two-dimensional graphene nanosheets MnNSG(NSG means N-and S-codoped graphene)as an active and durable OER catalyst with a low overpotential of 296 mV in alkaline media,compared to that of the benchmark IrO_(2) catalyst.Theoretical calculations and experimental measurements reveal that the Mn-N3S sites in the graphene matrix are the most active sites for the OER due to modified electronic structure of the Mn site by three nitrogen and one sulfur atoms coordination,which show lower theoretical overpotential than the Mn-N4 sites and over which the O–O formation step is the rate-determining step.

关 键 词：Mn-N-C N/S co-coordination oxygen evolution reaction single-atom catalyst theoretical calculations 

分 类 号：TQ426[化学工程]