A unified lattice–surface engineering strategy stabilizing oxygen redox in Li-rich cathodes for all-solid-state batteries
- 1Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Institute of New Energy, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), Fudan University, Shanghai 200433, China.
- 2School of Chemical Engineering, University of New South Wales, Sydney NSW, 2052, Australia.
- 3Department of Chemistry, AI Co-Research & Education for Innovative Drug Institute (AI-CRED Institute), Korea Advanced Institute of Science and Technology (KAIST), Daejeon 34141, Republic of Korea.
Abstract
Li-rich Mn-based layered oxides (LRMOs) are promising high-energy cathodes for all-solid-state batteries (ASSBs), but their application is limited by irreversible O₂ evolution during lattice O²⁻/O₂²⁻ redox and interfacial degradation at high voltages. Here we report a "coat-sinter-wash" synthetic strategy that simultaneously modulates bulk oxygen redox and stabilizes the cathode surface. An ammonium tungstate precursor is first coated onto LRMO particles. The subsequent sintering generates Li vacancies and enables W incorporation into the lattice, which acts as a "chemical rivet" and enhances the reversibility of lattice oxygen redox. A final washing step reconstructs the Li-deficient surface into an in-situ spinel layer, suppressing oxygen release from the surface and mitigating structural decomposition. The resulting ASSBs achieve remarkable cycling stability with 80% capacity retention over 500 cycles (0.5 C, 25°C) and an outstanding reversible capacity of 278.2 mAh g⁻¹ (0.1 C, 40°C). Furthermore, an all-solid-state pouch cell with Si anode demonstrates an areal capacity of 4.55 mAh cm⁻² and a high energy density of 543 Wh kg⁻¹. This work provides a scalable synthetic framework for stabilizing oxygen-redox cathodes in solid-state batteries.
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BibTeX
@article{ying2026unified,
title = {{A unified lattice–surface engineering strategy stabilizing oxygen redox in Li-rich cathodes for all-solid-state batteries}},
author = {Jiachen Ying and Gaohong Liu and Bingliang Wang and Yuwei Yang and Le Li and Linghao Deng and Guodong Li and Xing Zhou and Zhehan Zou and Yonggang Wang},
journal = {Science Advances},
year = {2026},
month = oct,
doi = {10.1126/sciadv.aei9538},
url = {https://www.science.org/doi/abs/10.1126/sciadv.aei9538},
note = {CC BY-NC},
}
RIS
TY - JOUR
TI - A unified lattice–surface engineering strategy stabilizing oxygen redox in Li-rich cathodes for all-solid-state batteries
AU - Jiachen Ying
AU - Gaohong Liu
AU - Bingliang Wang
AU - Yuwei Yang
AU - Le Li
AU - Linghao Deng
AU - Guodong Li
AU - Xing Zhou
AU - Zhehan Zou
AU - Yonggang Wang
PY - 2026
DA - 2026/10/28
JO - Science Advances
DO - 10.1126/sciadv.aei9538
UR - https://www.science.org/doi/abs/10.1126/sciadv.aei9538
AB - Li-rich Mn-based layered oxides (LRMOs) are promising high-energy cathodes for all-solid-state batteries (ASSBs), but their application is limited by irreversible O₂ evolution during lattice O²⁻/O₂²⁻ redox and interfacial degradation at high voltages. Here we report a "coat-sinter-wash" synthetic strategy that simultaneously modulates bulk oxygen redox and stabilizes the cathode surface. An ammonium tungstate precursor is first coated onto LRMO particles. The subsequent sintering generates Li vacancies and enables W incorporation into the lattice, which acts as a "chemical rivet" and enhances the reversibility of lattice oxygen redox. A final washing step reconstructs the Li-deficient surface into an in-situ spinel layer, suppressing oxygen release from the surface and mitigating structural decomposition. The resulting ASSBs achieve remarkable cycling stability with 80% capacity retention over 500 cycles (0.5 C, 25°C) and an outstanding reversible capacity of 278.2 mAh g⁻¹ (0.1 C, 40°C). Furthermore, an all-solid-state pouch cell with Si anode demonstrates an areal capacity of 4.55 mAh cm⁻² and a high energy density of 543 Wh kg⁻¹. This work provides a scalable synthetic framework for stabilizing oxygen-redox cathodes in solid-state batteries.
SN - 2375-2548
ER -