Assessing the Intrinsic Roles of Key Dopant Elements in High–Nickel Layered Oxide Cathodes in Lithium–Based Batteries

Cui, Zehao; Guo, Zezhou; Manthiram, Arumugam

doi:10.1002/aenm.202203853

Assessing the Intrinsic Roles of Key Dopant Elements in High–Nickel Layered Oxide Cathodes in Lithium–Based Batteries

Journal Article · Mon Feb 13 00:00:00 EST 2023 · Advanced Energy Materials

DOI:https://doi.org/10.1002/aenm.202203853· OSTI ID:2217449

Cui, Zehao ^[1]; Guo, Zezhou ^[2]; ^[2]

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

A rational compositional design is critical for utilizing LiNiO₂-based cathodes with Ni contents > 90% as promising next-generation cathode materials. Unfortunately, the lack of a fundamental understanding of the intrinsic roles of key elements, such as cobalt, manganese, and aluminum, makes the rational compositional design of high-Ni cathodes with a limited range of dopants (<10%) particularly challenging. Here, with 5% single-element doped cathodes, viz., LiNi_0.95Co_0.05O₂, LiNi_0.95Mn_0.05O₂, and LiNi_0.95Al_0.05O₂, along with undoped LiNiO₂ (LNO), the influences of the dopants are systematically examined through a control of cutoff charge energy density and a common practice of cutoff charge voltage. Comprehensive investigations into the electrochemical properties, combined with in-depth analyses of the structural and interfasial stabilities and electrolyte decomposition pathways through advanced characterizations, unveil the following: i) the intrinsic role of dopants regulates the cathode energy density or state-of-charge and, more critically, the occurrence of H2–H3 phase transition, which essentially dictates cyclability; ii) undoped LNO can be stabilized well with the avoidance of H2–H3 phase transition; and iii) Co provides more merits overall with an optimized electrochemical operating condition. Finally, this work provides guidance for the compositional design of high-energy-density high-Ni cathodes and sheds light on the challenges of removing Co.

View Accepted Manuscript (DOE)

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

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

Grant/Contract Number:: EE0007762

OSTI ID:: 2217449

Alternate ID(s):: OSTI ID: 1963359

Journal Information:: Advanced Energy Materials, Journal Name: Advanced Energy Materials Journal Issue: 12 Vol. 13; ISSN 1614-6832

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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