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Coherent Strain-Inhibiting Phase Construction of Lithium-Rich Manganese-Based Oxide Toward High Mechanochemical Stability

Journal Article · · Journal of the American Chemical Society
DOI:https://doi.org/10.1021/jacs.4c11385· OSTI ID:2575150
A layered lithium-rich manganese-based oxide cathode, containing $$R\overline{3}m$$ (LiTMO2, TM = Mn, Ni, Co) and $C2/m$ (Li2MnO3) nanodomains, utilizes both transition metals and oxygen redox to yield substantial energy density. However, the inherent heterogeneous nature and distinct nanodomain redox chemistries of layered lithium-rich oxides will inevitably cause pernicious lattice strain and structural displacement, which can hardly be eliminated by conventional doping or coating strategies and result in accelerated performance decay. Herein, we incorporate a strain-inhibiting perovskite phase coherently grown within the layered structure to effectively restrain the displacement and lattice strain during uneven Li-ion extraction. The enhanced mechanochemical stability of the designed cathode benefits the persistent structure and reversible oxygen redox, thereby achieving high initial Coulombic efficiency and stable cycling and voltage profiles. In conclusion, our approach of lattice engineering alleviates the strain and displacement caused by inhomogeneous reactivity between heterogeneous nanodomains and promotes the development of advanced cathode materials with long durability.
Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); National Natural Science Foundation of China (NSFC)
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
2575150
Journal Information:
Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 5 Vol. 147; ISSN 0002-7863; ISSN 1520-5126
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

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