A universal wet-chemistry synthesis of solid-state halide electrolytes for all-solid-state lithium-metal batteries

Changhong Wang; Jianwen Liang; Jing Luo; Jue Liu; Xiaona Li; Feipeng Zhao; Ruying Li; Huan Huang; Shangqian Zhao; Li Zhang; Jiantao Wang; Xueliang Sun

doi:10.1126/sciadv.abh1896

A universal wet-chemistry synthesis of solid-state halide electrolytes for all-solid-state lithium-metal batteries

Changhong Wang, Jianwen Liang, Jing Luo, Jue Liu, Xiaona Li, Feipeng Zhao, Ruying Li, Huan Huang, Shangqian Zhao, Li Zhang, Jiantao Wang, Xueliang Sun

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Abstract

Solid-state halide electrolytes have gained revived research interests owing to their high ionic conductivity and high-voltage stability. However, synthesizing halide electrolytes from a liquid phase is extremely challenging because of the vulnerability of metal halides to hydrolysis. In this work, ammonium-assisted wet chemistry is reported to synthesize various solid-state halide electrolytes with an exceptional ionic conductivity (>1 microsiemens per centimeter). Microstrain-induced localized microstructure change is found to be beneficial to lithium ion transport in halide electrolytes. Furthermore, the interfacial incompatibility between halide electrolytes and lithium metal is alleviated by transforming the mixed electronic/ionic conductive interface into a lithium ion–conductive interface. Such all-solid-state lithium-metal batteries (ASSLMBs) demonstrate a high initial coulombic efficiency of 98.1% based on lithium cobalt oxide and a high discharge capacity of 166.9 microampere hours per gram based on single-crystal LiNi_0.6Mn_0.2Co_0.2O₂. This work provides universal approaches in both material synthesis and interface design for developing halide-based ASSLMBs.

Original language	English
Article number	eabh1896
Journal	Science Advances
Volume	7
Issue number	37
DOIs	https://doi.org/10.1126/sciadv.abh1896
State	Published - Sep 2021

Funding

C.W. thanks Mitacs Accelerate Fellowships for their support. We thank S. Wang and Y. Mo from the University of Maryland for constructive discussion and suggestions. Funding: This work was supported by the Natural Sciences and Engineering Research Council of Canada (NSERC), Canada Research Chair Program (CRC), Canada Foundation for Innovation (CFI), Ontario Research Fund (ORF), China Automotive Battery Research Institute Co. Ltd., Glabat Solid-State Battery Inc., and University of Western Ontario. Neutron diffraction analysis conducted at the NOMAD beamlines at ORNL’s Spallation Neutron Source was sponsored by the Scientific User Facilities Division, Office of Basic Sciences, U.S. Department of Energy.

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abstract = "Solid-state halide electrolytes have gained revived research interests owing to their high ionic conductivity and high-voltage stability. However, synthesizing halide electrolytes from a liquid phase is extremely challenging because of the vulnerability of metal halides to hydrolysis. In this work, ammonium-assisted wet chemistry is reported to synthesize various solid-state halide electrolytes with an exceptional ionic conductivity (>1 microsiemens per centimeter). Microstrain-induced localized microstructure change is found to be beneficial to lithium ion transport in halide electrolytes. Furthermore, the interfacial incompatibility between halide electrolytes and lithium metal is alleviated by transforming the mixed electronic/ionic conductive interface into a lithium ion–conductive interface. Such all-solid-state lithium-metal batteries (ASSLMBs) demonstrate a high initial coulombic efficiency of 98.1% based on lithium cobalt oxide and a high discharge capacity of 166.9 microampere hours per gram based on single-crystal LiNi0.6Mn0.2Co0.2O2. This work provides universal approaches in both material synthesis and interface design for developing halide-based ASSLMBs.",

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AU - Li, Xiaona

AU - Zhao, Feipeng

AU - Li, Ruying

AU - Huang, Huan

AU - Zhao, Shangqian

AU - Zhang, Li

AU - Wang, Jiantao

AU - Sun, Xueliang

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N2 - Solid-state halide electrolytes have gained revived research interests owing to their high ionic conductivity and high-voltage stability. However, synthesizing halide electrolytes from a liquid phase is extremely challenging because of the vulnerability of metal halides to hydrolysis. In this work, ammonium-assisted wet chemistry is reported to synthesize various solid-state halide electrolytes with an exceptional ionic conductivity (>1 microsiemens per centimeter). Microstrain-induced localized microstructure change is found to be beneficial to lithium ion transport in halide electrolytes. Furthermore, the interfacial incompatibility between halide electrolytes and lithium metal is alleviated by transforming the mixed electronic/ionic conductive interface into a lithium ion–conductive interface. Such all-solid-state lithium-metal batteries (ASSLMBs) demonstrate a high initial coulombic efficiency of 98.1% based on lithium cobalt oxide and a high discharge capacity of 166.9 microampere hours per gram based on single-crystal LiNi0.6Mn0.2Co0.2O2. This work provides universal approaches in both material synthesis and interface design for developing halide-based ASSLMBs.

AB - Solid-state halide electrolytes have gained revived research interests owing to their high ionic conductivity and high-voltage stability. However, synthesizing halide electrolytes from a liquid phase is extremely challenging because of the vulnerability of metal halides to hydrolysis. In this work, ammonium-assisted wet chemistry is reported to synthesize various solid-state halide electrolytes with an exceptional ionic conductivity (>1 microsiemens per centimeter). Microstrain-induced localized microstructure change is found to be beneficial to lithium ion transport in halide electrolytes. Furthermore, the interfacial incompatibility between halide electrolytes and lithium metal is alleviated by transforming the mixed electronic/ionic conductive interface into a lithium ion–conductive interface. Such all-solid-state lithium-metal batteries (ASSLMBs) demonstrate a high initial coulombic efficiency of 98.1% based on lithium cobalt oxide and a high discharge capacity of 166.9 microampere hours per gram based on single-crystal LiNi0.6Mn0.2Co0.2O2. This work provides universal approaches in both material synthesis and interface design for developing halide-based ASSLMBs.

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A universal wet-chemistry synthesis of solid-state halide electrolytes for all-solid-state lithium-metal batteries

Abstract

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