Tuning Li occupancy and local structures for advanced Co-free Ni-rich positive electrodes

Hang Li (), Hao Liu, Shunrui Luo, Jordi Arbiol, Emmanuelle Suard, Thomas Bergfeldt, Alexander Missyul, Volodymyr Baran, Stefan Mangold, Yongchao Zhang, Weibo Hua, Michael Knapp, Helmut Ehrenberg, Feng Pan () and Sylvio Indris ()
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Hang Li: Peking University Shenzhen Graduate School
Hao Liu: Karlsruhe Institute of Technology (KIT)
Shunrui Luo: Bellaterra
Jordi Arbiol: Bellaterra
Emmanuelle Suard: Institute Laue-Langevin (ILL)
Thomas Bergfeldt: Karlsruhe Institute of Technology (KIT)
Alexander Missyul: CELLS-ALBA Synchrotron
Volodymyr Baran: Deutsches Elektronen-Synchrotron (DESY)
Stefan Mangold: Karlsruhe Institute of Technology (KIT)
Yongchao Zhang: Bellaterra
Weibo Hua: Xi’an Jiaotong University
Michael Knapp: Karlsruhe Institute of Technology (KIT)
Helmut Ehrenberg: Karlsruhe Institute of Technology (KIT)
Feng Pan: Peking University Shenzhen Graduate School
Sylvio Indris: Karlsruhe Institute of Technology (KIT)

Nature Communications, 2025, vol. 16, issue 1, 1-12

Abstract: Abstract Structure evolution and surface reactivity have long been regarded as the most crucial points for studying Ni-rich positive electrodes for Li-ion batteries. Unfortunately, the influence of Li occupancy as a single factor on electro-chemomechanical stability has been overlooked and is missing, owing to the challenge of Li determination in the lattice. Here, a comprehensive analysis reveals different Li occupancies and related structural domains (Ni/Li exchange, LiaXOb, Li/Mn/X(Ni) ordering domains, X = Nb5+, W6+, and Mo6+) by using a combination of Li-sensitive characterization techniques. By introducing a Li-regulation strategy, the relative ratio of each domain is effectively tuned in the Ni-rich positive electrodes. Through tuning, two specific positive electrodes are designed, exhibiting notable improvement in battery cyclability. The specific Li structural units induce significant changes in redox mechanisms. This Li-occupancy-tuning approach highlights the necessity of focusing on Li distribution and opens up ideas for designing advanced Ni-rich positive electrodes with high durability.

Date: 2025
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DOI: 10.1038/s41467-025-57063-7

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