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author：

Huang, Youzhang (Huang, Youzhang.) [1] | Li, Jiantao (Li, Jiantao.) [2] | Zhang, Yinggan (Zhang, Yinggan.) [3] | Lin, Liang (Lin, Liang.) [4] | Sun, Zhefei (Sun, Zhefei.) [5] | Gao, Guiyang (Gao, Guiyang.) [6] | Sa, Baisheng (Sa, Baisheng.) [7] | Wang, Laisen (Wang, Laisen.) [8] | Ma, Lu (Ma, Lu.) [9] | Lee, Sungsik (Lee, Sungsik.) [10] | Wang, Ming-Sheng (Wang, Ming-Sheng.) [11] | Peng, Dong-Liang (Peng, Dong-Liang.) [12] | Amine, Khalil (Amine, Khalil.) [13] | Xie, Qingshui (Xie, Qingshui.) [14]

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EI

Abstract：

Sluggish　redox　kinetics　and　dendrite　growth　perplex　the　fulfillment　of　efficient　electrochemistry　in　lithium-sulfur　(Li-S)　batteries.　The　complicated　sulfur　phase　transformation　and　sulfur/lithium　diversity　kinetics　necessitate　an　all-inclusive　approach　in　catalyst　design.　Herein,　a　compatible　mediator　with　nanoscale-asymmetric-size　configuration　by　integrating　Co　single　atoms　and　defective　CoTe2-x　(CoSA-CoTe2-x@NHCF)　is　elaborately　developed　for　regulating　sulfur/lithium　electrochemistry　synchronously.　Substantial　electrochemistry　and　theoretical　analyses　reveal　that　CoTe2-x　exhibits　higher　catalytic　activity　in　long-chain　polysulfide　transformation　and　Li2S　decomposition,　while　monodispersed　Co　sites　are　more　effective　in　boosting　sulfur　reduction　kinetics　to　regulate　Li2S　deposition.　Such　cascade　catalysis　endows　CoSA-CoTe2-x@NHCF　with　the　all-around　service　of　＇trapping-conversion-recuperation＇　for　sulfur　species　during　the　whole　redox　reaction.　Furthermore,　it　is　demonstrated　by　in　situ　transmission　electron　microscopy　that　initially　formed　electronic-conductive　Co　and　ionic-conductive　Li2Te　provide　sufficient　lithiophilic　sites　to　regulate　homogeneous　Li　plating　and　stripping　with　markedly　suppressed　dendrite　growth.　Consequently,　by　coupling　the　CoSA-CoTe2-x@NHCF　interlayer　and　Li@CoSA-CoTe2-x@NHCF　anode,　the　constructed　Li-S　full　batteries　deliver　superior　cycling　stability　and　rate　performance,　and　the　flexible　pouch　cell　exhibits　stable　cycling　performance　at　0.3　C.　The　gained　insights　into　the　synergistic　effect　of　asymmetric-size　structures　pave　the　way　for　the　integrated　catalyst　design　in　advanced　Li-S　systems.　©　2025　UChicago　Argonne,　LLC,　Operator　of　Argonne　National　Laboratory.　Published　by　American　Chemical　Society.

Keyword：

Bioremediation Dendrites (metallography) Hard facing High resolution transmission electron microscopy Lithium compounds Lithium-ion batteries Lithium sulfur batteries Redox reactions Sulfur compounds Sulfur determination

Community：

  • [ 1 ] [Huang, Youzhang]State Key Laboratory of Physical Chemistry of Solid Surface, Fujian Key Laboratory of Surface and Interface Engineering for High Performance Materials, College of Materials, Xiamen University, Xiamen; 361005, China
  • [ 2 ] [Li, Jiantao]Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont; IL; 60439, United States
  • [ 3 ] [Zhang, Yinggan]State Key Laboratory of Physical Chemistry of Solid Surface, Fujian Key Laboratory of Surface and Interface Engineering for High Performance Materials, College of Materials, Xiamen University, Xiamen; 361005, China
  • [ 4 ] [Lin, Liang]State Key Laboratory of Physical Chemistry of Solid Surface, Fujian Key Laboratory of Surface and Interface Engineering for High Performance Materials, College of Materials, Xiamen University, Xiamen; 361005, China
  • [ 5 ] [Sun, Zhefei]State Key Laboratory of Physical Chemistry of Solid Surface, Fujian Key Laboratory of Surface and Interface Engineering for High Performance Materials, College of Materials, Xiamen University, Xiamen; 361005, China
  • [ 6 ] [Gao, Guiyang]State Key Laboratory of Physical Chemistry of Solid Surface, Fujian Key Laboratory of Surface and Interface Engineering for High Performance Materials, College of Materials, Xiamen University, Xiamen; 361005, China
  • [ 7 ] [Sa, Baisheng]Multiscale Computational Materials Facility, College of Materials Science and Engineering, Fuzhou University, Fuzhou; 350100, China
  • [ 8 ] [Wang, Laisen]State Key Laboratory of Physical Chemistry of Solid Surface, Fujian Key Laboratory of Surface and Interface Engineering for High Performance Materials, College of Materials, Xiamen University, Xiamen; 361005, China
  • [ 9 ] [Ma, Lu]National Synchrotron Light Source II (NSLS-II), Brookhaven National Laboratory, Upton; NY; 11973, United States
  • [ 10 ] [Lee, Sungsik]X-ray Science Division, Argonne National Laboratory, Lemont; IL; 60439, United States
  • [ 11 ] [Wang, Ming-Sheng]State Key Laboratory of Physical Chemistry of Solid Surface, Fujian Key Laboratory of Surface and Interface Engineering for High Performance Materials, College of Materials, Xiamen University, Xiamen; 361005, China
  • [ 12 ] [Peng, Dong-Liang]State Key Laboratory of Physical Chemistry of Solid Surface, Fujian Key Laboratory of Surface and Interface Engineering for High Performance Materials, College of Materials, Xiamen University, Xiamen; 361005, China
  • [ 13 ] [Amine, Khalil]Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont; IL; 60439, United States
  • [ 14 ] [Amine, Khalil]Pritzker School of Molecular Engineering, The University of Chicago, Chicago; IL; 60637, United States
  • [ 15 ] [Xie, Qingshui]State Key Laboratory of Physical Chemistry of Solid Surface, Fujian Key Laboratory of Surface and Interface Engineering for High Performance Materials, College of Materials, Xiamen University, Xiamen; 361005, China

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Journal of the American Chemical Society

ISSN： 0002-7863

Year： 2025

Issue： 6

Volume： 147

Page： 4752-4765

1 4 . 5 0 0

JCR@2023

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ESI Highly Cited Papers on the List： 0 Unfold All

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