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Nano Research 2023, 16(4): 5080-5086 https://doi.org/10.1007/s12274-021-3683-6
Research Article | Issue | Published: 13 July 2021

A homogenous solid polymer electrolyte prepared by facile spray drying method is used for room-temperature solid lithium metal batteries

Show Author's Information Zehao Zhou1,§,  Tong Sun3,§,  Jin Cui1,  Xiu Shen2,  Chuan Shi1( ),  Shuang Cao3,  Jinbao Zhao2( )
College of Physics, Qingdao University, Qingdao 266071, China
Collaborative Innovation Center of Chemistry for Energy Materials, State Key Lab of Physical Chemistry of Solid Surfaces, State-Province Joint Engineering Laboratory of Power Source Technology for New Energy Vehicle, Engineering Research Center of Electrochemical Technology, Ministry of Education, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China
College of Chemistry and Chemical Engineering, Qingdao University, Qingdao 266071, China

§ Zehao Zhou and Tong Sun contributed equally to this work.

Keywords:
spray drying, solid polymer electrolytes, homogenous dispersion, solid lithium batteries, surface electric field, polyvinylidene fluoride/Li6.4La3Zr1.4Ta0.6O12 (PVDF/LLZTO)
Cite this article:
Zhou Z, Sun T, Cui J, et al. A homogenous solid polymer electrolyte prepared by facile spray drying method is used for room-temperature solid lithium metal batteries. Nano Research, 2023, 16(4): 5080-5086. https://doi.org/10.1007/s12274-021-3683-6
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Abstract Full text Electronic supplementary material About this article

The aggregation of inorganic particles with high mass ratio will form a heterogeneous electric field in the solid polymer electrolytes (SPEs), which is difficult to be compatible with lithium anode, leading to inadequate ionic conductivity. Herein, a facile spray drying method is adopted to increase the mass ratio of inorganic particles and solve the aggregation problems of fillers simultaneously. The polyvinylidene fluoride (PVDF) with lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) covers the surface of each Li6.4La3Zr1.4Ta0.6O12 (LLZTO) granules during the nebulization process, then forming flat solid electrolytes via layer-by-layer deposition. Characterized by the atomic force microscope, the obtained solid electrolytes achieve a homogenous dispersion of Young’s modulus and surface electric field. As a result, the as-prepared SPEs present high tensile strength of 7.1 MPa, high ionic conductivity of 1.86 × 10−4 S·cm−1 at room temperature, and wide electrochemical window up to 5.0 V, demonstrating increased mechanical strength and uniform lithium-ion migration channels for SPEs. Thanks to the as-prepared SPEs, the lithium-symmetrical cells show a highly stable Li plating/stripping cycling for over 1,000 h at 0.1 mA·cm−2. The corresponding Li/LCoO2 batteries also present good rate capability and excellent cyclic performance with capacity retention of 80% after 100 cycles at room temperature.


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Abstract
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Electronic supplementary material
About this article

A homogenous solid polymer electrolyte prepared by facile spray drying method is used for room-temperature solid lithium metal batteries

Show Author's information Zehao Zhou1,§, Tong Sun3,§, Jin Cui1, Xiu Shen2, Chuan Shi1( ), Shuang Cao3, Jinbao Zhao2( )
College of Physics, Qingdao University, Qingdao 266071, China
Collaborative Innovation Center of Chemistry for Energy Materials, State Key Lab of Physical Chemistry of Solid Surfaces, State-Province Joint Engineering Laboratory of Power Source Technology for New Energy Vehicle, Engineering Research Center of Electrochemical Technology, Ministry of Education, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China
College of Chemistry and Chemical Engineering, Qingdao University, Qingdao 266071, China

§ Zehao Zhou and Tong Sun contributed equally to this work.

Abstract

The aggregation of inorganic particles with high mass ratio will form a heterogeneous electric field in the solid polymer electrolytes (SPEs), which is difficult to be compatible with lithium anode, leading to inadequate ionic conductivity. Herein, a facile spray drying method is adopted to increase the mass ratio of inorganic particles and solve the aggregation problems of fillers simultaneously. The polyvinylidene fluoride (PVDF) with lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) covers the surface of each Li6.4La3Zr1.4Ta0.6O12 (LLZTO) granules during the nebulization process, then forming flat solid electrolytes via layer-by-layer deposition. Characterized by the atomic force microscope, the obtained solid electrolytes achieve a homogenous dispersion of Young’s modulus and surface electric field. As a result, the as-prepared SPEs present high tensile strength of 7.1 MPa, high ionic conductivity of 1.86 × 10−4 S·cm−1 at room temperature, and wide electrochemical window up to 5.0 V, demonstrating increased mechanical strength and uniform lithium-ion migration channels for SPEs. Thanks to the as-prepared SPEs, the lithium-symmetrical cells show a highly stable Li plating/stripping cycling for over 1,000 h at 0.1 mA·cm−2. The corresponding Li/LCoO2 batteries also present good rate capability and excellent cyclic performance with capacity retention of 80% after 100 cycles at room temperature.

Keywords: spray drying, solid polymer electrolytes, homogenous dispersion, solid lithium batteries, surface electric field, polyvinylidene fluoride/Li6.4La3Zr1.4Ta0.6O12 (PVDF/LLZTO)

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Publication history
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Acknowledgements

Publication history

Received: 13 April 2021
Revised: 06 June 2021
Accepted: 16 June 2021
Published: 13 July 2021
Issue date: April 2023

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© Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2021

Acknowledgements

Acknowledgements

We gratefully acknowledge the financial support from the National Natural Science Foundation of China (No. 21805147).

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