Protective Coating of Single-Crystalline Ni-Rich Cathode Enables Fast Charging in All-Solid-State Batteries.
basic_science · Level V
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- Record sourced from PubMed, PMID 39879526.
- Also identified by DOI 10.1021/acsnano.4c14322.
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Abstract
Improving interfacial stability between cathode active material (CAM) and solid electrolyte (SE) is vital for developing high-performance all-solid-state batteries (ASSBs), with compatibility issues among the cell components representing a major challenge. CAM surface coating with a chemically inert ion conductor is a promising approach to suppress side reactions occurring at the cathode interfaces. Another strategy to mitigate mechanical degradation involves utilizing single-crystalline particle morphologies. Their more robust bulk structure and lower tortuosity for charge transport, compared to polycrystalline (PC) CAMs, can significantly enhance cyclability in ASSBs. Herein, we coated a LiNbO<sub>3</sub> protective layer onto the free surface of quasi single-crystalline LiNi<sub>0.83</sub>Co<sub>0.12</sub>Mn<sub>0.05</sub>O<sub>2</sub> (SC83) particles. Pellet-stack ASSB cells using the LiNbO<sub>3</sub>@SC83 CAM and argyrodite Li<sub>6</sub>PS<sub>5</sub>Cl as SE showed a capacity retention of 88% after 1000 cycles at the 1 C rate, compared to only 71% for the uncoated counterpart and far superior to that of LiNbO<sub>3</sub>@PC83 (30%). The effectiveness of LiNbO<sub>3</sub> coating and the SC-NCM nature in mitigating electro-chemo-mechanical degradation was studied by combining modeling and physical/electrochemical characterizations. We demonstrate that the capacity decay at fast charge is due primarily to the mechanical degradation of CAM particles, while it is strongly determined by CAM|SE interfacial reactions under slow-charging conditions.