Tuning Li occupancy and local structures for advanced Co-free Ni-rich positive electrodes
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, Li<sub>a</sub>XO<sub>b</sub>, Li/Mn/X(Ni) ordering domains, X = Nb<sup>5+</sup>, W<sup>6+</sup>, and Mo<sup>6+</sup>) 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.
Authors
- Helmut Ehrenberg (ORCID: https://orcid.org/0000-0002-5134-7130)
- Shunrui Luo (ORCID: https://orcid.org/0000-0003-4910-4604)
- Jordi Arbiol (ORCID: https://orcid.org/0000-0002-0695-1726)
- Emmanuelle Suard (ORCID: https://orcid.org/0000-0001-5966-5929)
- Sylvio Indris (ORCID: https://orcid.org/0000-0002-5100-113X)
- Michael Knapp (ORCID: https://orcid.org/0000-0003-0091-8463)
- Volodymyr Baran (ORCID: https://orcid.org/0000-0003-2379-3632)
- Feng Ming Pan (ORCID: https://orcid.org/0000-0002-8216-1339)
- Weibo Hua (ORCID: https://orcid.org/0000-0001-5372-4422)
- Alexander Missyul (ORCID: https://orcid.org/0000-0002-0577-4481)
- Thomas Bergfeldt (ORCID: https://orcid.org/0000-0003-4595-7968)
- Hang Li (ORCID: https://orcid.org/0000-0002-6738-7938)
- Hao Liu (ORCID: https://orcid.org/0000-0003-0266-9472)
- Yongchao Zhang (ORCID: https://orcid.org/0000-0001-8931-6738)
- Stefan Mangold (ORCID: https://orcid.org/0000-0003-2298-6985)
Institutions
- Karlsruhe Institute of Technology (DE)
- Institució Catalana de Recerca i Estudis Avançats (ES)
- Peking University (CN)
- ALBA Synchrotron (Spain) (ES)
- Deutsches Elektronen-Synchrotron DESY (DE)
- Institut Langevin (FR)
- Institut Català de Nanociència i Nanotecnologia (ES)
- Institut Català de Ciències del Clima (ES)
- Peking University Shenzhen Hospital (CN)
- Université Mohammed VI Polytechnique (MA)
- Xi'an Jiaotong University (CN)
Publication Details
- Journal
- Nature Communications
- Published
- 2025-03-05
- DOI
- https://doi.org/10.1038/s41467-025-57063-7
- Citations
- 18
- Primary Topic
- Advancements in Battery Materials
- Type
- article
- Field-Weighted Citation Impact
- 13.15
Funders
- Center of Excellence for Learning in Education, Science and Technology
- Centres de Recerca de Catalunya
- Institut Català de Nanociència i Nanotecnologia
- European Commission
- European Synchrotron Radiation Facility
- Generalitat de Catalunya
- Peking University
- Deutsches Elektronen-Synchrotron
- European Regional Development Fund
- Agencia Estatal de Investigación
- Soft Science Research Project of Guangdong Province
- Basic and Applied Basic Research Foundation of Guangdong Province