Improving Ionic Conductivity with Bimodal-Sized Li                         7                         La                         3                         Zr                         2                         O                         12                          Fillers for Composite Polymer Electrolytes

Yan Sun; Xiaowen Zhan; Jiazhi Hu; Yikai Wang; Shuang Gao; Yuhua Shen; Yang Tse Cheng

doi:10.1021/acsami.8b21770

Improving Ionic Conductivity with Bimodal-Sized Li ₇ La ₃ Zr ₂ O ₁₂ Fillers for Composite Polymer Electrolytes

Yan Sun, Xiaowen Zhan, Jiazhi Hu, Yikai Wang, Shuang Gao, Yuhua Shen, Yang Tse Cheng

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

93 Scopus citations

Abstract

Ceramic-polymer composite electrolytes (CPEs) are being explored to achieve both high ionic conductivity and mechanical flexibility. Here, we show that, by incorporating 10 wt % (3 vol %) mixed-sized fillers of Li ₇ La ₃ Zr ₂ O ₁₂ (LLZO) doped with Nb/Al, the roomerature ionic conductivity of a polyvinylidene fluoride (PVDF)-LiClO ₄ -based composite can be as high as 2.6 × 10 ^-4 S/cm, which is 1 order of magnitude higher than that with nano- or micrometer-sized LLZO particles as fillers. The CPE also shows a high lithium-ion transference number of 0.682, a stable and low Li/CPE interfacial resistance, and good mechanical properties favorable for all-solid-state lithium-ion battery applications. X-ray photoelectron spectroscopy and Raman analysis demonstrate that the LLZO fillers of all sizes interact with PVDF and LiClO ₄ . High packing density (i.e., lower porosity) and long conducting pathways are believed responsible for the excellent performance of the composite electrolyte filled with mixed-sized ionically conducting ceramic particles.

Original language	English
Pages (from-to)	12467-12475
Number of pages	9
Journal	ACS Applied Materials and Interfaces
Volume	11
Issue number	13
DOIs	https://doi.org/10.1021/acsami.8b21770
State	Published - Apr 3 2019

Bibliographical note

Funding Information:
Y.S. and Y.S. gratefully acknowledge the financial support from the National Science Foundation of China no. 21671001 and 21571002. X.Z., J.H., Y.W., S.G., and Y.-T.C. gratefully acknowledge the financial support from the National Science Foundation (award no: 1355438, Powering the Kentucky Bioeconomy for a Sustainable Future). X.Z. would like to thank the Department of Chemical and Materials Engineering at the University of Kentucky for its partial financial support of this work. Y.S. would like to acknowledge the support from the China Scholarship Council. The authors would like to thank Namal Wanninayake of the University of Kentucky for helping with Raman measurements.

Publisher Copyright:
© 2019 American Chemical Society.

Keywords

Li La Zr O
ceramicâpolymer interactions
composite polymer electrolytes
ionic conductivity
lithium batteries

ASJC Scopus subject areas

Materials Science (all)

UN SDGs

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

Access to Document

10.1021/acsami.8b21770

Cite this

Sun, Y., Zhan, X., Hu, J., Wang, Y., Gao, S., Shen, Y., & Cheng, Y. T. (2019). Improving Ionic Conductivity with Bimodal-Sized Li ₇ La ₃ Zr ₂ O ₁₂ Fillers for Composite Polymer Electrolytes ACS Applied Materials and Interfaces, 11(13), 12467-12475. https://doi.org/10.1021/acsami.8b21770

Sun, Yan ; Zhan, Xiaowen ; Hu, Jiazhi et al. / Improving Ionic Conductivity with Bimodal-Sized Li ₇ La ₃ Zr ₂ O ₁₂ Fillers for Composite Polymer Electrolytes In: ACS Applied Materials and Interfaces. 2019 ; Vol. 11, No. 13. pp. 12467-12475.

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title = " Improving Ionic Conductivity with Bimodal-Sized Li 7 La 3 Zr 2 O 12 Fillers for Composite Polymer Electrolytes ",

abstract = " Ceramic-polymer composite electrolytes (CPEs) are being explored to achieve both high ionic conductivity and mechanical flexibility. Here, we show that, by incorporating 10 wt % (3 vol %) mixed-sized fillers of Li 7 La 3 Zr 2 O 12 (LLZO) doped with Nb/Al, the roomerature ionic conductivity of a polyvinylidene fluoride (PVDF)-LiClO 4 -based composite can be as high as 2.6 × 10 -4 S/cm, which is 1 order of magnitude higher than that with nano- or micrometer-sized LLZO particles as fillers. The CPE also shows a high lithium-ion transference number of 0.682, a stable and low Li/CPE interfacial resistance, and good mechanical properties favorable for all-solid-state lithium-ion battery applications. X-ray photoelectron spectroscopy and Raman analysis demonstrate that the LLZO fillers of all sizes interact with PVDF and LiClO 4 . High packing density (i.e., lower porosity) and long conducting pathways are believed responsible for the excellent performance of the composite electrolyte filled with mixed-sized ionically conducting ceramic particles. ",

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author = "Yan Sun and Xiaowen Zhan and Jiazhi Hu and Yikai Wang and Shuang Gao and Yuhua Shen and Cheng, {Yang Tse}",

note = "Funding Information: Y.S. and Y.S. gratefully acknowledge the financial support from the National Science Foundation of China no. 21671001 and 21571002. X.Z., J.H., Y.W., S.G., and Y.-T.C. gratefully acknowledge the financial support from the National Science Foundation (award no: 1355438, Powering the Kentucky Bioeconomy for a Sustainable Future). X.Z. would like to thank the Department of Chemical and Materials Engineering at the University of Kentucky for its partial financial support of this work. Y.S. would like to acknowledge the support from the China Scholarship Council. The authors would like to thank Namal Wanninayake of the University of Kentucky for helping with Raman measurements. Publisher Copyright: {\textcopyright} 2019 American Chemical Society.",

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Sun, Y, Zhan, X, Hu, J, Wang, Y, Gao, S, Shen, Y & Cheng, YT 2019, ' Improving Ionic Conductivity with Bimodal-Sized Li ₇ La ₃ Zr ₂ O ₁₂ Fillers for Composite Polymer Electrolytes ', ACS Applied Materials and Interfaces, vol. 11, no. 13, pp. 12467-12475. https://doi.org/10.1021/acsami.8b21770

Improving Ionic Conductivity with Bimodal-Sized Li ₇ La ₃ Zr ₂ O ₁₂ Fillers for Composite Polymer Electrolytes . / Sun, Yan; Zhan, Xiaowen; Hu, Jiazhi et al.
In: ACS Applied Materials and Interfaces, Vol. 11, No. 13, 03.04.2019, p. 12467-12475.

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

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AU - Gao, Shuang

AU - Shen, Yuhua

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N2 - Ceramic-polymer composite electrolytes (CPEs) are being explored to achieve both high ionic conductivity and mechanical flexibility. Here, we show that, by incorporating 10 wt % (3 vol %) mixed-sized fillers of Li 7 La 3 Zr 2 O 12 (LLZO) doped with Nb/Al, the roomerature ionic conductivity of a polyvinylidene fluoride (PVDF)-LiClO 4 -based composite can be as high as 2.6 × 10 -4 S/cm, which is 1 order of magnitude higher than that with nano- or micrometer-sized LLZO particles as fillers. The CPE also shows a high lithium-ion transference number of 0.682, a stable and low Li/CPE interfacial resistance, and good mechanical properties favorable for all-solid-state lithium-ion battery applications. X-ray photoelectron spectroscopy and Raman analysis demonstrate that the LLZO fillers of all sizes interact with PVDF and LiClO 4 . High packing density (i.e., lower porosity) and long conducting pathways are believed responsible for the excellent performance of the composite electrolyte filled with mixed-sized ionically conducting ceramic particles.

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Sun Y, Zhan X, Hu J, Wang Y, Gao S, Shen Y et al. Improving Ionic Conductivity with Bimodal-Sized Li ₇ La ₃ Zr ₂ O ₁₂ Fillers for Composite Polymer Electrolytes ACS Applied Materials and Interfaces. 2019 Apr 3;11(13):12467-12475. doi: 10.1021/acsami.8b21770