Atomic Manganese Manipulating Polysulfide Speciation Pathway for Room-Temperature Na-S Batteries

作     者：Hong Zhang Mingli Wang Xiang-Long Huang Songtao Lu Ke Lu Xiaohong Wu 

作者机构：School of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbinHeilongjiang 150001 Institutes of Physical Science and Information TechnologyAnhui UniversityHefeiAnhui 230601 Institute of Fundamental and Frontier SciencesUniversity of Electronic Science and Technology of ChinaChengdu 610054 

出 版 物：《CCS Chemistry》 (中国化学会会刊（英文）)

年 卷 期：2024年第6卷第9期

页      面：2289-2304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] 

基　　金：financially supported by the Natural Scientific Foundation of China(grant nos.22109001 and 22208335) the Postdoctoral Fellowship Program of CPSF(grant no.GZB20230950) the Heilongjiang Postdoctoral Science Foundation(grant no.LBH-Z23187) the Jiangsu Key Laboratory for Carbon-Based Functional Materials&Devices,Soochow University(grant no.KJS2308) startup funds provided to H.Z.from the Harbin Institute of Technology 

主　　题：single-atom manganese catalysts polysulfide manipulation reaction kinetics bidirectional catalysts sodium-sulfur batteries 

摘      要：Sluggish polysulfide redox kinetics,especially the high energy barrier of rate-determining short-chain polysulfide conversion and the high activation barrier of Na_(2)S decomposition during sulfur recovery,compromise the full potential of rechargeable Na-S *** we construct the hierarchical sandwich-structured carbon matrix with atomically dispersed Mn-N4 Lewis acidic sites,taking advantage of their bidirectional electrocatalytic behavior toward interface-mediated reversible sulfur *** and theoretical results reveal that the spatial confinement and catalytic effects facilitated via strong Lewis acid-base electron interactions synergistically manipulate the low kinetically direct Na_(2)S_(4) to Na_(2)S conversion,and the formation of Mn-S bond minimizes the energy barrier of Na_(2)S electrochemical activation during battery recharging,thereby rendering a reversible and tunable polysulfide speciation ***,the degradation of the Na-S cell is due to the depletion of metal anode rather than the loss of active sulfur species and/or aggregation of inactive dead *** expected,the S@Mn/NC cathode delivers outstanding rate capability and ultrahigh cycling ***,a proof-of-concept pouch cell was also demonstrated capable of delivering an energy density up to 840 Wh kgcathode−*** tunable sulfur redox electrochemistry invoked by the bidirectional monodispersed Mn catalytic hot spots facilitates the efficient polysulfide speciation for practical Na-S cells.