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

CCS Chemistry 2024年第9期6卷 2289-2304页

作者： Hong Zhang Mingli Wang Xiang-Long Huang Songtao Lu Ke Lu Xiaohong Wu School of Chemistry and Chemical Engineering Harbin Institute of TechnologyHarbinHeilongjiang 150001 Institutes of Physical Science and Information Technology Anhui UniversityHefeiAnhui 230601 Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of ChinaChengdu 610054

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.

关键词： single-atom manganese catalysts polysulfide manipulation reaction kinetics bidirectional catalysts sodium-sulfur batteries

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