Energizing Robust Sulfur/Lithium Electrochemistry via Nanoscale-Asymmetric-Size Synergism - Details

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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.

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[ 1 ] [Huang Y.]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 J.]Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, 60439, IL, United States
[ 3 ] [Zhang Y.]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 L.]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 Z.]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 G.]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 B.]Multiscale Computational Materials Facility, College of Materials Science and Engineering, Fuzhou University, Fuzhou, 350100, China
[ 8 ] [Wang L.]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 L.]National Synchrotron Light Source II (NSLS-II), Brookhaven National Laboratory, Upton, 11973, NY, United States
[ 10 ] [Lee S.]X-ray Science Division, Argonne National Laboratory, Lemont, 60439, IL, United States
[ 11 ] [Wang M.-S.]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 D.-L.]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 K.]Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, 60439, IL, United States
[ 14 ] [Amine K.]Pritzker School of Molecular Engineering, The University of Chicago, Chicago, 60637, IL, United States
[ 15 ] [Xie Q.]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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