Cobalt-free composite-structured cathodes with lithium-stoichiometry control for sustainable lithium-ion batteries

Ke Chen, Pallab Barai, Ozgenur Kahvecioglu, Lijun Wu, Krzysztof Z. Pupek, Mingyuan Ge, Lu Ma, Steven N. Ehrlich, Hui Zhong, Yimei Zhu, Venkat Srinivasan, Jianming Bai () and Feng Wang ()
Additional contact information
Ke Chen: Brookhaven National Laboratory
Pallab Barai: Argonne National Laboratory
Ozgenur Kahvecioglu: Argonne National Laboratory
Lijun Wu: Brookhaven National Laboratory
Krzysztof Z. Pupek: Argonne National Laboratory
Mingyuan Ge: Brookhaven National Laboratory
Lu Ma: Brookhaven National Laboratory
Steven N. Ehrlich: Brookhaven National Laboratory
Hui Zhong: Stony Brook University
Yimei Zhu: Brookhaven National Laboratory
Venkat Srinivasan: Argonne National Laboratory
Jianming Bai: Brookhaven National Laboratory
Feng Wang: Brookhaven National Laboratory

Nature Communications, 2024, vol. 15, issue 1, 1-10

Abstract: Abstract Lithium-ion batteries play a crucial role in decarbonizing transportation and power grids, but their reliance on high-cost, earth-scarce cobalt in the commonly employed high-energy layered Li(NiMnCo)O2 cathodes raises supply-chain and sustainability concerns. Despite numerous attempts to address this challenge, eliminating Co from Li(NiMnCo)O2 remains elusive, as doing so detrimentally affects its layering and cycling stability. Here, we report on the rational stoichiometry control in synthesizing Li-deficient composite-structured LiNi0.95Mn0.05O2, comprising intergrown layered and rocksalt phases, which outperforms traditional layered counterparts. Through multiscale-correlated experimental characterization and computational modeling on the calcination process, we unveil the role of Li-deficiency in suppressing the rocksalt-to-layered phase transformation and crystal growth, leading to small-sized composites with the desired low anisotropic lattice expansion/contraction during charging and discharging. As a consequence, Li-deficient LiNi0.95Mn0.05O2 delivers 90% first-cycle Coulombic efficiency, 90% capacity retention, and close-to-zero voltage fade for 100 deep cycles, showing its potential as a Co-free cathode for sustainable Li-ion batteries.

Date: 2024
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DOI: 10.1038/s41467-023-44583-3

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