Delineating the Roles of Mn, Al, and Co by Comparing Three Layered Oxide Cathodes with the Same Nickel Content of 70% for Lithium-Ion Batteries

Yi, Michael; Li, Wangda; Manthiram, Arumugam

doi:10.1021/acs.chemmater.1c03322

Delineating the Roles of Mn, Al, and Co by Comparing Three Layered Oxide Cathodes with the Same Nickel Content of 70% for Lithium-Ion Batteries

Journal Article · Sun Jan 09 23:00:00 EST 2022 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.1c03322· OSTI ID:1972445

Yi, Michael ^[1]; ^[2]; ^[2]

Univ. of Texas at Austin, TX (United States); University of Texas at Austin
Univ. of Texas at Austin, TX (United States)

High-nickel layered oxides continue to prevail in the energy storage market as the frontmost cathode candidates for next-generation lithium-ion batteries. Demand and development of LiNi_1–x–yMn_xCo_yO₂ (NMC) and LiNi_1–x–yCo_xAl_yO₂ (NCA) cathodes are rampantly increasing, particularly for the electric vehicle (EV) industry. However, the continued presence of cobalt in NMC and NCA cathodes raises global concerns due to geopolitical and ethical issues attributed to Co sourcing. We herein introduce a novel cobalt-free, high-nickel cathode LiNi_0.7Mn_0.25Al_0.05O₂ (NMA70) and benchmark it against Co-containing LiNi_0.7Mn_0.15Co_0.15O₂ (NMC70) as well as Co- and Al-free LiNi_0.7Mn_0.3O₂ (NM70) cathodes with equivalent 70% Ni contents that are all synthesized in-house. NMA70 displays a high initial C/10 capacity of 210 mA h g^–1, matching that of NMC70 in half cells with a cutoff voltage of 4.5 V. NMA70 also exhibits an impressive high-voltage full cell cycling performance with a cutoff voltage of 4.4 V with a nearly identical capacity retention of 83% compared to that of 82% for NMC70 after 300 cycles. Postmortem X-ray photoelectron spectroscopy (XPS), high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), and electron energy loss spectroscopy (EELS) analyses indicate a thinner cathode–electrolyte interface (CEI) developed in NMA70 compared to that in NM70 and unveil a more robust solid-electrolyte interface (SEI) passivation on the graphite anode among all samples. The benefits of Al doping are additionally highlighted with enhanced high-voltage CEI and thermal stabilities in NMA70. Furthermore, this work assesses the roles of Mn, Al, and Co to demonstrate both the practicality and feasibility of synthesizing cobalt-free, high-nickel cathodes that are promising alternatives to current NMC- and NCA-based cathodes.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Texas at Austin, TX (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO)

Grant/Contract Number:: EE0008445

OSTI ID:: 1972445

Alternate ID(s):: OSTI ID: 2326342

Journal Information:: Chemistry of Materials, Journal Name: Chemistry of Materials Journal Issue: 2 Vol. 34; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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