Unraveling the Roles of Dissolved Mn(2+) and Its Impact on the Electrode-Electrolyte Interface under Realistic Conditions - Details

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NMC532　(LiNi0.5Mn0.3Co0.2O2)　is　a　cost-effective　and　structurally　stable　cathode　material　that　is　widely　used　in　batteries.　Despite　its　stability,　it　undergoes　irreversible　phase　transitions　and　transition　metal　(TM)　dissolution　during　long-term　cycling,　which　significantly　impacts　cell　performance.　This　study　pioneered　a　methodology　to　investigate　the　solid　electrolyte　interface　(SEI)　layers　in　depth,　employing　advanced　analytical　techniques:　time-of-flight　secondary　ion　mass　spectrometry　(TOF-SIMS)　and　cluster　analysis.　By　utilizing　these　techniques,　we　specifically　examined　the　impact　of　Mn　dissolution　on　the　interface　evolution　of　graphite　during　calendar　degradations.　Additionally,　we　explored　the　relationship　between　Mn　dissolution　and　cell　performance　in　a　graphite||NMC532　pouch　cell.　The　results　demonstrate　that　the　competition　between　Mn　dissolution　and　electrolyte　depletion　governs　cell　degradation.　In　particular,　Mn　dissolution　accelerates　the　decomposition　of　the　electrolyte,　ultimately　causing　SEI　layer　growth.　These　findings　provide　a　deeper　understanding　of　battery　performance　and　degradation　mechanisms.　©　2024　American　Chemical　Society.

Keyword：

Cathodes Cluster analysis Cobalt compounds Degradation Dissolution Graphite Ions Lithium compounds Lithium-ion batteries Manganese Manganese compounds Nickel compounds Secondary emission Secondary ion mass spectrometry Solid electrolytes

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[ 1 ] [Xie, Yuxiang]State Key Laboratory of Physical Chemistry of Solid Surfaces, and Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen; 361005, China
[ 2 ] [Li, Wei]Reliability Safety Department & Mechanism Simulation, Contemporary Amperex Technology Company Limited, Ningde; 352100, China
[ 3 ] [Hu, Huan]Institute of Applied Genomics, Fuzhou University, Fuzhou; 350108, China
[ 4 ] [Shi, Chen-Guang]State Key Laboratory of Physical Chemistry of Solid Surfaces, and Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen; 361005, China
[ 5 ] [Hong, Yu-Hao]Tan Kah Kee Innovation Laboratory, Xiamen; 361102, China
[ 6 ] [Dai, Peng]State Key Laboratory of Physical Chemistry of Solid Surfaces, and Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen; 361005, China
[ 7 ] [Lin, Zhen]Reliability Safety Department & Mechanism Simulation, Contemporary Amperex Technology Company Limited, Ningde; 352100, China
[ 8 ] [Sha, Ying]Reliability Safety Department & Mechanism Simulation, Contemporary Amperex Technology Company Limited, Ningde; 352100, China
[ 9 ] [Wang, Junfeng]Reliability Safety Department & Mechanism Simulation, Contemporary Amperex Technology Company Limited, Ningde; 352100, China
[ 10 ] [Xie, Lan]Reliability Safety Department & Mechanism Simulation, Contemporary Amperex Technology Company Limited, Ningde; 352100, China
[ 11 ] [Wu, Kai]Reliability Safety Department & Mechanism Simulation, Contemporary Amperex Technology Company Limited, Ningde; 352100, China
[ 12 ] [Huang, Ling]State Key Laboratory of Physical Chemistry of Solid Surfaces, and Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen; 361005, China
[ 13 ] [Sun, Shi-Gang]State Key Laboratory of Physical Chemistry of Solid Surfaces, and Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen; 361005, China

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Source ：

ACS Sustainable Chemistry and Engineering

ISSN： 2168-0485

Year： 2024

Issue： 17

Volume： 12

Page： 6529-6538

7 . 1 0 0

JCR@2023

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