A Series of Ternary Metal Chloride Superionic Conductors for High-Performance All-Solid-State Lithium Batteries

Jianwen Liang; Eveline van der Maas; Jing Luo; Xiaona Li; Ning Chen; Keegan R. Adair; Weihan Li; Junjie Li; Yongfeng Hu; Jue Liu; Li Zhang; Shangqian Zhao; Shigang Lu; Jiantao Wang; Huan Huang; Wenxuan Zhao; Steven Parnell; Ronald I. Smith; Swapna Ganapathy; Marnix Wagemaker; Xueliang Sun

doi:10.1002/aenm.202103921

A Series of Ternary Metal Chloride Superionic Conductors for High-Performance All-Solid-State Lithium Batteries

Jianwen Liang, Eveline van der Maas, Jing Luo, Xiaona Li, Ning Chen, Keegan R. Adair, Weihan Li, Junjie Li, Yongfeng Hu, Jue Liu, Li Zhang, Shangqian Zhao, Shigang Lu, Jiantao Wang, Huan Huang, Wenxuan Zhao, Steven Parnell, Ronald I. Smith, Swapna Ganapathy, Marnix WagemakerXueliang Sun

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Abstract

Understanding the relationship between structure, ionic conductivity, and synthesis is the key to the development of superionic conductors. Here, a series of Li_3-3_xM₁₊_xCl₆ (−0.14 < x ≤ 0.5, M = Tb, Dy, Ho, Y, Er, Tm) solid electrolytes with orthorhombic and trigonal structures are reported. The orthorhombic phase of Li–M–Cl shows an approximately one order of magnitude increase in ionic conductivities when compared to their trigonal phase. Using the Li–Ho–Cl components as an example, their structures, phase transition, ionic conductivity, and electrochemical stability are studied. Molecular dynamics simulations reveal the facile diffusion in the z-direction in the orthorhombic structure, rationalizing the improved ionic conductivities. All-solid-state batteries of NMC811/Li_2.73Ho_1.09Cl₆/In demonstrate excellent electrochemical performance at both 25 and −10 °C. As relevant to the vast number of isostructural halide electrolytes, the present structure control strategy guides the design of halide superionic conductors.

Original language	English
Article number	2103921
Journal	Advanced Energy Materials
Volume	12
Issue number	21
DOIs	https://doi.org/10.1002/aenm.202103921
State	Published - Jun 2 2022

Funding

J.L., E.v.d.M., and J.L. contributed equally to this work. This research was supported by the Natural Sciences and Engineering Research Council of Canada (NSERC), Canada Research Chair Program (CRC), Canada Foundation for Innovation (CFI), GLABAT Solid‐State Battery Inc., China Automotive Battery Research Institute Co. Ltd, Ontario Research Fund, the Canada Light Source at University of Saskatchewan (CLS), Interdisciplinary Development Initiatives (IDI) by Western University, Canada MITACS fellow, and University of Western Ontario. Financial support was greatly acknowledged from the Netherlands Organization for Scientific Research (NWO) under the VICI Grant No. 16122. The authors also appreciate the help of the beamline scientist of HXMA (Dr. Weifeng Chen) and SXRMB (Dr. Mohsen Shakouri, Dr. Qunfeng Xiao, and Dr. Alisa Paterson) beamline at Canadian Light Source. The authors thank the UK Science and Technology Facilities Council (STFC) for provision of Xpress Access neutron beamtime at ISIS. [ 59 ] J.L., E.v.d.M., and J.L. contributed equally to this work. This research was supported by the Natural Sciences and Engineering Research Council of Canada (NSERC), Canada Research Chair Program (CRC), Canada Foundation for Innovation (CFI), GLABAT Solid-State Battery Inc., China Automotive Battery Research Institute Co. Ltd, Ontario Research Fund, the Canada Light Source at University of Saskatchewan (CLS), Interdisciplinary Development Initiatives (IDI) by Western University, Canada MITACS fellow, and University of Western Ontario. Financial support was greatly acknowledged from the Netherlands Organization for Scientific Research (NWO) under the VICI Grant No. 16122. The authors also appreciate the help of the beamline scientist of HXMA (Dr. Weifeng Chen) and SXRMB (Dr. Mohsen Shakouri, Dr. Qunfeng Xiao, and Dr. Alisa Paterson) beamline at Canadian Light Source. The authors thank the UK Science and Technology Facilities Council (STFC) for provision of Xpress Access neutron beamtime at ISIS.[59]

Keywords

all-solid-state Li batteries
energy storage
halides
solid-state electrolytes
superionic conductors

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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Liang, J., van der Maas, E., Luo, J., Li, X., Chen, N., Adair, K. R., Li, W., Li, J., Hu, Y., Liu, J., Zhang, L., Zhao, S., Lu, S., Wang, J., Huang, H., Zhao, W., Parnell, S., Smith, R. I., Ganapathy, S., ... Sun, X. (2022). A Series of Ternary Metal Chloride Superionic Conductors for High-Performance All-Solid-State Lithium Batteries. Advanced Energy Materials, 12(21), Article 2103921. https://doi.org/10.1002/aenm.202103921

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title = "A Series of Ternary Metal Chloride Superionic Conductors for High-Performance All-Solid-State Lithium Batteries",

abstract = "Understanding the relationship between structure, ionic conductivity, and synthesis is the key to the development of superionic conductors. Here, a series of Li3-3xM1+xCl6 (−0.14 < x ≤ 0.5, M = Tb, Dy, Ho, Y, Er, Tm) solid electrolytes with orthorhombic and trigonal structures are reported. The orthorhombic phase of Li–M–Cl shows an approximately one order of magnitude increase in ionic conductivities when compared to their trigonal phase. Using the Li–Ho–Cl components as an example, their structures, phase transition, ionic conductivity, and electrochemical stability are studied. Molecular dynamics simulations reveal the facile diffusion in the z-direction in the orthorhombic structure, rationalizing the improved ionic conductivities. All-solid-state batteries of NMC811/Li2.73Ho1.09Cl6/In demonstrate excellent electrochemical performance at both 25 and −10 °C. As relevant to the vast number of isostructural halide electrolytes, the present structure control strategy guides the design of halide superionic conductors.",

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author = "Jianwen Liang and {van der Maas}, Eveline and Jing Luo and Xiaona Li and Ning Chen and Adair, {Keegan R.} and Weihan Li and Junjie Li and Yongfeng Hu and Jue Liu and Li Zhang and Shangqian Zhao and Shigang Lu and Jiantao Wang and Huan Huang and Wenxuan Zhao and Steven Parnell and Smith, {Ronald I.} and Swapna Ganapathy and Marnix Wagemaker and Xueliang Sun",

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year = "2022",

month = jun,

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doi = "10.1002/aenm.202103921",

language = "English",

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Liang, J, van der Maas, E, Luo, J, Li, X, Chen, N, Adair, KR, Li, W, Li, J, Hu, Y, Liu, J, Zhang, L, Zhao, S, Lu, S, Wang, J, Huang, H, Zhao, W, Parnell, S, Smith, RI, Ganapathy, S, Wagemaker, M & Sun, X 2022, 'A Series of Ternary Metal Chloride Superionic Conductors for High-Performance All-Solid-State Lithium Batteries', Advanced Energy Materials, vol. 12, no. 21, 2103921. https://doi.org/10.1002/aenm.202103921

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T1 - A Series of Ternary Metal Chloride Superionic Conductors for High-Performance All-Solid-State Lithium Batteries

AU - Liang, Jianwen

AU - van der Maas, Eveline

AU - Luo, Jing

AU - Li, Xiaona

AU - Chen, Ning

AU - Adair, Keegan R.

AU - Li, Weihan

AU - Li, Junjie

AU - Hu, Yongfeng

AU - Liu, Jue

AU - Zhang, Li

AU - Zhao, Shangqian

AU - Lu, Shigang

AU - Wang, Jiantao

AU - Huang, Huan

AU - Zhao, Wenxuan

AU - Parnell, Steven

AU - Smith, Ronald I.

AU - Ganapathy, Swapna

AU - Wagemaker, Marnix

AU - Sun, Xueliang

PY - 2022/6/2

Y1 - 2022/6/2

N2 - Understanding the relationship between structure, ionic conductivity, and synthesis is the key to the development of superionic conductors. Here, a series of Li3-3xM1+xCl6 (−0.14 < x ≤ 0.5, M = Tb, Dy, Ho, Y, Er, Tm) solid electrolytes with orthorhombic and trigonal structures are reported. The orthorhombic phase of Li–M–Cl shows an approximately one order of magnitude increase in ionic conductivities when compared to their trigonal phase. Using the Li–Ho–Cl components as an example, their structures, phase transition, ionic conductivity, and electrochemical stability are studied. Molecular dynamics simulations reveal the facile diffusion in the z-direction in the orthorhombic structure, rationalizing the improved ionic conductivities. All-solid-state batteries of NMC811/Li2.73Ho1.09Cl6/In demonstrate excellent electrochemical performance at both 25 and −10 °C. As relevant to the vast number of isostructural halide electrolytes, the present structure control strategy guides the design of halide superionic conductors.

AB - Understanding the relationship between structure, ionic conductivity, and synthesis is the key to the development of superionic conductors. Here, a series of Li3-3xM1+xCl6 (−0.14 < x ≤ 0.5, M = Tb, Dy, Ho, Y, Er, Tm) solid electrolytes with orthorhombic and trigonal structures are reported. The orthorhombic phase of Li–M–Cl shows an approximately one order of magnitude increase in ionic conductivities when compared to their trigonal phase. Using the Li–Ho–Cl components as an example, their structures, phase transition, ionic conductivity, and electrochemical stability are studied. Molecular dynamics simulations reveal the facile diffusion in the z-direction in the orthorhombic structure, rationalizing the improved ionic conductivities. All-solid-state batteries of NMC811/Li2.73Ho1.09Cl6/In demonstrate excellent electrochemical performance at both 25 and −10 °C. As relevant to the vast number of isostructural halide electrolytes, the present structure control strategy guides the design of halide superionic conductors.

KW - all-solid-state Li batteries

KW - energy storage

KW - halides

KW - solid-state electrolytes

KW - superionic conductors

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U2 - 10.1002/aenm.202103921

DO - 10.1002/aenm.202103921

M3 - Article

AN - SCOPUS:85127594179

SN - 1614-6832

VL - 12

JO - Advanced Energy Materials

JF - Advanced Energy Materials

IS - 21

M1 - 2103921

ER -

A Series of Ternary Metal Chloride Superionic Conductors for High-Performance All-Solid-State Lithium Batteries

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Keywords

UN SDGs

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