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(De)Lithiation Mechanism of Hierarchically Layered LiNi$_{1/3}$Co$_{1/3}$Mn$_{1/3}$O$_{2}$ Cathodes during High-Voltage Cycling

Hua, Weibo; Schwarz, Björn; Knapp, Michael; Senyshyn, Anatoliy; Missiul, Alkesandr; Mu, Xiaoke; Wang, Suning; Kübel, Christian; Binder, Joachim R.; Indris, Sylvio; Ehrenberg, Helmut

In view of the requirements for high-energy lithium ion batteries (LIBs), hierarchically layered LiNi1/3Co1/3Mn1/3O2 (NCM111) cathode materials have been prepared using a hydroxide coprecipitation method and subsequent high-temperature solid-state reaction. The diffraction results show that the synthesized NCM111 has a well-defined layered hexagonal structure. The initial specific discharge capacity of a Li/NCM111 cell is 204.5 mAh g−1 at a current density of 28 mA g−1 between 2.7 and 4.8 V. However, the cell suffers from poor capacity retention over extended charge-discharge cycles. The structural evolution of NCM111 electrode during electrochemical cycling is carefully investigated by in situ high-resolution synchrotron radiation diffraction. It is found that the nanodomain formation of a layered hexagonal phase H3 and a cubic spinel phase after charging to voltages above 4.6 V is the main source for the structural collapse in c direction and the poor cycling performance. This process is accompanied by the removal of oxygen, the transition metal (TM) migration and the crack generation in the nanodomains of the primary particles. T ... mehr

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Verlagsausgabe §
DOI: 10.5445/IR/1000087647
Veröffentlicht am 20.11.2018
Zugehörige Institution(en) am KIT Institut für Nanotechnologie (INT)
Institut für Angewandte Materialien - Energiespeichersysteme (IAM-ESS)
Helmholtz-Institut Ulm (HIU)
Karlsruhe Nano Micro Facility (KNMF)
Publikationstyp Zeitschriftenaufsatz
Jahr 2019
Sprache Englisch
Identifikator ISSN: 0013-4651
KITopen-ID: 1000087647
HGF-Programm 37.01.02 (POF III, LK 01)
Erschienen in Journal of the Electrochemical Society
Band 166
Heft 3
Seiten A5025–A5032
Vorab online veröffentlicht am 06.11.2018
Schlagworte Batteries - Lithium; high voltage cycling; in situ diffraction; structural evolution
Nachgewiesen in Web of Science
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