Molding of Li5.5PS4.5Cl1.5 Particles Based on Regulating Li+ Transport for All-Solid-State Li Metal Battery

Guanwu Li; Dong Wang; Bo Gao; Changru Rong; Xuepeng Li; Zixiao Zhang; Jiayu Wang; Jinyi Zhao; Xiaofei Yang; Jian Wang; Xinyan Zhou; Hongzhen Lin; Wei Zhang; Yingze Song; Zhi Chang; Yunfeng Jiang; Xing Ou; Weitao Zheng

doi:10.1002/anie.202520479

Molding of Li_5.5PS_4.5Cl_1.5 Particles Based on Regulating Li⁺ Transport for All-Solid-State Li Metal Battery

Angew Chem Int Ed Engl. 2026 Jan 22;65(4):e20479. doi: 10.1002/anie.202520479. Epub 2025 Dec 3.

Authors

Guanwu Li¹, Dong Wang¹, Bo Gao¹, Changru Rong², Xuepeng Li¹, Zixiao Zhang¹, Jiayu Wang¹, Jinyi Zhao¹, Xiaofei Yang³, Jian Wang^{4

5}, Xinyan Zhou¹, Hongzhen Lin⁴, Wei Zhang¹, Yingze Song⁶, Zhi Chang⁷, Yunfeng Jiang², Xing Ou⁸, Weitao Zheng¹

Affiliations

¹ State Key Laboratory of High Pressure and Superhard Materials, and School of Materials Science and Engineering, and Jilin Provincial International Cooperation Key Laboratory of High-Efficiency Clean Energy Materials, and Electron Microscopy Center, and International Center of Future Science, Jilin University, Changchun, 130013, P. R. China.
² General Research and Development Institute, China FAW Corporation Limited, Changchun, 130013, P. R. China.
³ Key Laboratory of Long-Duration and Large-Scale Energy Storage, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, China.
⁴ i-Lab & CAS Key Laboratory of Nanophotonic Materials and Devices, Suzhou Institute of Nano-tech and Nano-bionics, Chinese Academy of Sciences, Suzhou, 215123, P. R. China.
⁵ Karlsruhe Institute of Technology (KIT), Karlsruhe, D76021, Germany.
⁶ School of Materials and Chemistry, State Key Laboratory of Environment-Friendly Energy Materials, Southwest University of Science and Technology, Mianyang, 621010, China.
⁷ School of Materials Science and Engineering, Central South University, Changsha, Hunan, 410083, China.
⁸ Hunan Province Key Laboratory of Chemical Power Source, School of Materials Science and Engineering, College of Chemistry and Chemical Engineering, Central South University, Changsha, 410083, P. R. China.

PMID: 41332340
DOI: 10.1002/anie.202520479

Abstract

All-solid-state Li metal batteries (ASSLBs) are coming with sulfide solid-state electrolytes (S-SSEs) for superior Li⁺ conductivity, but irregular particles and interfaces lead to disorder Li⁺ flux in S-SSEs that hinder pure Li as an anode. Specially, its mesoscopic structure cannot be adequately described by average size, making it difficult to analyze Li⁺ flux effectively. Herein, a model is constructed on the molding of Li_5.5PS_4.5Cl_1.5 (LPSC) particles and defined size as the number (N) and consistency (σ) to evaluate their effects on Li⁺ transfer and concentration uniformity. Through machine learning of calculation data (Li⁺ concentration with N and σ) and experimental results, excessive interfaces can hinder Li⁺ transport and local aggregation of irregular interfaces leads to uneven ion transport. Therefore, a particle size gradient S-SSEs (induced by different size LPSC particles) is predicted to achieve fast and uniform Li⁺ transport. Subsequently, this designed S-SSE is applied in ASSLBs, which can complete a 1000 h cycle with capacity retention exceeding 80%. This study elucidates that the long cycle ASSLBs can be achieved by adjusting the molding of LPSC particles. Specifically, it demonstrates that the Li⁺ flux of the whole S-SSEs can be optimized through gradient size design.

Keywords: All‐solid‐state battery; Li metal anode; Li+ flux; Molding of Li5.5PS4.5Cl1.5 particles.

Abstract

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