Large-scale manufacturing sulfide superionic conductor for advancing all-solid-state batteries

Shuo Wang; Chenjie Lou; Xinbin Wu; Jing Lin; Ajay Gautam; Shenghao Li; Jielei Huang; Zhu Cheng; Shengnan Zhang; Xin Zhang; Florian Strauss; Torsten Brezesinski; Guoqiang Luo; Mingxue Tang; Yang Shen; Yuanhua Lin; Ce Wen Nan

doi:10.1016/j.matt.2025.102135

Large-scale manufacturing sulfide superionic conductor for advancing all-solid-state batteries

Shuo Wang
, Chenjie Lou
, Xinbin Wu
, Jing Lin
, Ajay Gautam
, Shenghao Li
, Jielei Huang
, Zhu Cheng
, Shengnan Zhang
, Xin Zhang
, Florian Strauss
, Torsten Brezesinski
, Guoqiang Luo
, Mingxue Tang
, Yang Shen
, Yuanhua Lin
, Ce Wen Nan

Powder Diffraction

Research output: Contribution to journal › Article › peer-review

30 Scopus citations

Abstract

Lithium argyrodites with high ionic conductivities are favorable solid electrolytes (SEs) for all-solid-state batteries (ASSBs). However, their low preparation efficiency and poor cycling performance hinder their large-scale applications. In this work, we demonstrate successful large-scale production (over 1 kg per batch for the first time) of Li_5.5PS_4.5Cl_0.75Br_0.75 (LPSCB) by fast dry mixing followed by annealing, which presents high room temperature ionic conductivities of 13 mS cm⁻¹ for cold-pressed and 25 mS cm⁻¹ for sintered pellets. Combining neutron powder diffraction and ⁶Li → ⁷Li tracer-exchange nuclear magnetic resonance (NMR) spectroscopy measurements, we show that intercage jumps frequently occur through the 48h-16e-48h pathway in LPSCB, promoting the overall lithium conduction. The assembled ASSBs using LPSCB and a LiNi_0.83Co_0.11Mn_0.06O₂ electrode can be cycled for over 2,500 cycles at a 0.5 C rate and 1,800 cycles at a 2 C rate without any capacity degradation. Our results will accelerate the commercialization of sulfide SE for ASSBs.

Original language	English
Article number	102135
Journal	Matter
Volume	8
Issue number	9
DOIs	https://doi.org/10.1016/j.matt.2025.102135
State	Published - Sep 3 2025

Funding

C.-W.N. acknowledges the Natural Science Foundation of China (grant no. 52388201 ). S.W. acknowledges the Natural Science Foundation of China (grant no. 52302305 ) and the Natural Science Foundation Exploration Program of Wuhan (Morning Light Plan) (grant no. 202401jc0089 ) and support from the Tong Xiang Advanced New Materials Institute . M.T. acknowledges the Natural Science Foundation of China (grant no. 22090043 ). J.L. acknowledges the Fonds der Chemischen Industrie (FCI) for financial support. F.S. is grateful to the Federal Ministry of Education and Research (BMBF) for funding within the project MELLi ( 03XP0447 ). This research used resources at the PEARL neutron source, Delft University of Technology. The authors thank Dr. Xinxin Tan for providing the s-NCM83 cathode material, Yahao Mu for conducting the Raman measurements, and Dr. Indu Dhiman for assistance with the NPD measurements.

Keywords

all-solid-state battery
large-scale preparation
MAP 5: Improvement
NMR
stable cycling
sulfide solid electrolyte

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10.1016/j.matt.2025.102135

Cite this

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title = "Large-scale manufacturing sulfide superionic conductor for advancing all-solid-state batteries",

abstract = "Lithium argyrodites with high ionic conductivities are favorable solid electrolytes (SEs) for all-solid-state batteries (ASSBs). However, their low preparation efficiency and poor cycling performance hinder their large-scale applications. In this work, we demonstrate successful large-scale production (over 1 kg per batch for the first time) of Li5.5PS4.5Cl0.75Br0.75 (LPSCB) by fast dry mixing followed by annealing, which presents high room temperature ionic conductivities of 13 mS cm−1 for cold-pressed and 25 mS cm−1 for sintered pellets. Combining neutron powder diffraction and 6Li → 7Li tracer-exchange nuclear magnetic resonance (NMR) spectroscopy measurements, we show that intercage jumps frequently occur through the 48h-16e-48h pathway in LPSCB, promoting the overall lithium conduction. The assembled ASSBs using LPSCB and a LiNi0.83Co0.11Mn0.06O2 electrode can be cycled for over 2,500 cycles at a 0.5 C rate and 1,800 cycles at a 2 C rate without any capacity degradation. Our results will accelerate the commercialization of sulfide SE for ASSBs.",

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author = "Shuo Wang and Chenjie Lou and Xinbin Wu and Jing Lin and Ajay Gautam and Shenghao Li and Jielei Huang and Zhu Cheng and Shengnan Zhang and Xin Zhang and Florian Strauss and Torsten Brezesinski and Guoqiang Luo and Mingxue Tang and Yang Shen and Yuanhua Lin and Nan, \{Ce Wen\}",

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AU - Wang, Shuo

AU - Lou, Chenjie

AU - Wu, Xinbin

AU - Lin, Jing

AU - Gautam, Ajay

AU - Li, Shenghao

AU - Huang, Jielei

AU - Cheng, Zhu

AU - Zhang, Shengnan

AU - Zhang, Xin

AU - Strauss, Florian

AU - Brezesinski, Torsten

AU - Luo, Guoqiang

AU - Tang, Mingxue

AU - Shen, Yang

AU - Lin, Yuanhua

AU - Nan, Ce Wen

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N2 - Lithium argyrodites with high ionic conductivities are favorable solid electrolytes (SEs) for all-solid-state batteries (ASSBs). However, their low preparation efficiency and poor cycling performance hinder their large-scale applications. In this work, we demonstrate successful large-scale production (over 1 kg per batch for the first time) of Li5.5PS4.5Cl0.75Br0.75 (LPSCB) by fast dry mixing followed by annealing, which presents high room temperature ionic conductivities of 13 mS cm−1 for cold-pressed and 25 mS cm−1 for sintered pellets. Combining neutron powder diffraction and 6Li → 7Li tracer-exchange nuclear magnetic resonance (NMR) spectroscopy measurements, we show that intercage jumps frequently occur through the 48h-16e-48h pathway in LPSCB, promoting the overall lithium conduction. The assembled ASSBs using LPSCB and a LiNi0.83Co0.11Mn0.06O2 electrode can be cycled for over 2,500 cycles at a 0.5 C rate and 1,800 cycles at a 2 C rate without any capacity degradation. Our results will accelerate the commercialization of sulfide SE for ASSBs.

AB - Lithium argyrodites with high ionic conductivities are favorable solid electrolytes (SEs) for all-solid-state batteries (ASSBs). However, their low preparation efficiency and poor cycling performance hinder their large-scale applications. In this work, we demonstrate successful large-scale production (over 1 kg per batch for the first time) of Li5.5PS4.5Cl0.75Br0.75 (LPSCB) by fast dry mixing followed by annealing, which presents high room temperature ionic conductivities of 13 mS cm−1 for cold-pressed and 25 mS cm−1 for sintered pellets. Combining neutron powder diffraction and 6Li → 7Li tracer-exchange nuclear magnetic resonance (NMR) spectroscopy measurements, we show that intercage jumps frequently occur through the 48h-16e-48h pathway in LPSCB, promoting the overall lithium conduction. The assembled ASSBs using LPSCB and a LiNi0.83Co0.11Mn0.06O2 electrode can be cycled for over 2,500 cycles at a 0.5 C rate and 1,800 cycles at a 2 C rate without any capacity degradation. Our results will accelerate the commercialization of sulfide SE for ASSBs.

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KW - MAP 5: Improvement

KW - NMR

KW - stable cycling

KW - sulfide solid electrolyte

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Large-scale manufacturing sulfide superionic conductor for advancing all-solid-state batteries

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Keywords

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