Lattice and Local Electronic Structure Modulation Enables Ultra-Long-Life Li-Rich Cathode Materials - Details

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Effectively　alleviating　severe　performance　deterioration　including　rapid　capacity　decay　and　continuous　voltage　fading　of　Li-rich　layered　oxide　(LLO)　cathodes　by　suppressing　the　irreversible　oxygen　release　and　transition　metal　(TM)　migration　is　a　critical　challenge　during　prolonged　cycling.　Herein,　we　report　a　Sb-doped　LLO　(SLLO)　cathode　with　shortened　TMoct-TMoct　distance　and　modulated　local　electronic　structure,　which　can　significantly　enhance　the　oxygen　vacancy　formation　energy　and　TM　migration　energy　barriers.　Therefore,　the　SLLO　cathode　showcases　an　impressive　energy　density　of　1052　Wh　kg-1　at　0.2　C　and　an　outstanding　rate　capability　of　214　mAh　g-1　at　5　C　with　a　remarkable　capacity　retention　of　79.2%　even　after　1000　cycles.　It　should　be　pointed　out　that　it　exhibits　greatly　enhanced　voltage　stability　with　an　outstanding　voltage　retention　of　86.2%　after　cycling　1600　times　at　10　C.　This　work　provides　a　prototype　for　significantly　enhancing　the　reversibility　in　electrochemical　reactions　of　high-capacity　layered　cathode　materials.　©　2024　UChicago　Argonne,　LLC,　Operator　of　Argonne　National　Laboratory.　Published　by　American　Chemical　Society.

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[ 1 ] [Han X.]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 ] [Wu R.]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
[ 3 ] [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
[ 4 ] [Li J.]Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, 60439, IL, United States
[ 5 ] [Fan M.]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 ] [Wang 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
[ 7 ] [Liu 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
[ 8 ] [Li 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
[ 9 ] [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
[ 10 ] [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
[ 11 ] [Sa B.]Multiscale Computational Materials Facility, College of Materials Science and Engineering, Fuzhou University, Fuzhou, 350100, China
[ 12 ] [Lin J.]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 ] [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
[ 14 ] [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
[ 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
[ 16 ] [Amine K.]Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, 60439, IL, United States

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ACS Energy Letters

ISSN： 2380-8195

Year： 2024

Issue： 7

Volume： 9

Page： 3219-3226

1 9 . 5 0 0

JCR@2023

CAS Journal Grade：1

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