Spin engineering of single-site metal catalysts

作     者：Zichuang Li Ruguang Ma Qiangjian Ju Qian Liu Lijia Liu Yufang Zhu Minghui Yang Jiacheng Wang 

作者机构：State Key Laboratory of High-Performance Ceramics and Superfine MicrostructureShanghai Institute of CeramicsChinese Academy of Sciences1295 Dingxi RoadShanghai 200050China Center of Materials Science and Optoelectronics EngineeringUniversity of Chinese Academy of SciencesBeijing 100049China School of Materials Science and EngineeringSuzhou University of Science and Technology99 Xuefu RoadSuzhou 215009China Department of ChemistryWestern University1151 Richmond StreetLondonON N6A 5B7Canada Ningbo Institute of Materials Technology and EngineeringChinese Academy of Sciences1219 Zhongguan West RoadNingbo 315201China Hebei Provincial Key Laboratory of Inorganic Nonmetallic MaterialsCollege of Materials Science and EngineeringNorth China University of Science and TechnologyTangshan 063210China 

出 版 物：《The Innovation》 (创新（英文）)

年 卷 期：2022年第3卷第4期

页      面：96-103页

核心收录：

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] 0702[理学-物理学] 

基　　金：support from the National Natural Science Foundation of China(grants 92163117,52072389,and 52172058) State Key Laboratory of ASIC&Sys-tem(grant 2020KF002) J.W.thanks the Program of Shanghai Academic Research Leader(grant 20XD1424300)for financial support.LL.acknowledges support from the Discovery Program of the Natural Sciences and Engineering Research Council of Canada(NSERC,grant DG RGPIN-2020-06675) Use of the Advanced Photon Source was supported by the U.S.Department of Energy,Office of Science,Office of Basic Energy Sciences,under contract DE-AC02-06CH11357 Technical support from APS beamline scientists Dr.George E.Ster-binsky and Dr.Tianpin Wu,and from TLS beamline scientist Dr.Lo-Yueh Chang,is greatly appreciated 

主　　题：kinetics attracting faster 

摘      要：Single-site metal atoms(SMAs)on supports are attracting extensive interest as new catalytic systems because of maximized atom utilization and superior ***,rational design of configuration-optimized SMAs with high activity from the perspectives of fundamental electron spin is highly ***,N-coordinated Fe single atoms are successfully distributed over axial carbon micropores to form dangling-FeN4 centers(d-FeN4).This unique d-FeN4 demonstrates much higher intrinsic activity toward oxygen reduction reaction(ORR)in HClO4 than FeN4 without micropore underneath and commercial Pt/*** theoretical calculation and electronic structure characterization imply that d-FeN4 endows central Fe with medium spin(t2g 4 eg 1),which provides a spin channel for electron transition compared with FeN4 with low *** leads to the facile formation of the singlet state of oxygen-containing species from triplet oxygen during the ORR,thus showing faster kinetics than *** work provides an in-depth understanding of spin tuning on SMAs for advanced energy catalysis.