High Ionic Conductivity and Transfer Number of Composite Solid Electrolyte for Advanced Lithium Battery by Synergetic Effect of Halloysite Nanotube and High-entropy Zeolitic Imidazolate Frameworks

Yong-Li Du; Yong-Fan Cao; Zhen-Zhu Cao; Li-Ying Wang; Shao-Hua Luo

doi:10.1007/s10118-026-3738-y

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High Ionic Conductivity and Transfer Number of Composite Solid Electrolyte for Advanced Lithium Battery by Synergetic Effect of Halloysite Nanotube and High-entropy Zeolitic Imidazolate Frameworks

RESEARCH ARTICLE | Updated：2026-09-23

- High Ionic Conductivity and Transfer Number of Composite Solid Electrolyte for Advanced Lithium Battery by Synergetic Effect of Halloysite Nanotube and High-entropy Zeolitic Imidazolate Frameworks
- Chinese Journal of Polymer Science Vol. 44, Issue 10, Pages: 3513-3527(2026)
- Affiliations：
  
  a.Chemical Engineering College, Inner Mongolia University of Technology, Hohhot 010051, China
  b.Department of Physics and Electronic Information Engineering, Lyuliang University, Lvliang 033001, China
  c.Hebei Key Laboratory of Dielectric and Electrolyte Functional Material, Northeastern University at Qinhuangdao, Qinhuangdao 066003, China
- Author bio：
  
  czz03@imut.edu.cn (Z.Z.C.)
  wly2004@imut.edu.cn (L.Y.W.)
- Funds：
- DOI：10.1007/s10118-026-3738-y
  CLC：
- Received：02 April 2026，
  
  Accepted：05 May 2026，
  
  Online First：06 July 2026，
  
  Published：05 October 2026
- Accepted：
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Du, Y. L.; Cao, Y. F.; Cao, Z. Z.; Wang, L. Y.; Luo, S. H. High ionic conductivity and transfer number of composite solid electrolyte for advanced lithium battery by synergetic effect of halloysite nanotube and high-entropy zeolitic imidazolate frameworks. Chinese J. Polym. Sci. 2026, 44, 3513–3527

Yong-Li Du, Yong-Fan Cao, Zhen-Zhu Cao, et al. High Ionic Conductivity and Transfer Number of Composite Solid Electrolyte for Advanced Lithium Battery by Synergetic Effect of Halloysite Nanotube and High-entropy Zeolitic Imidazolate Frameworks[J]. Chinese Journal of Polymer Science, 2026, 44(10): 3513-3527.
Du, Y. L.; Cao, Y. F.; Cao, Z. Z.; Wang, L. Y.; Luo, S. H. High ionic conductivity and transfer number of composite solid electrolyte for advanced lithium battery by synergetic effect of halloysite nanotube and high-entropy zeolitic imidazolate frameworks. Chinese J. Polym. Sci. 2026, 44, 3513–3527 DOI： 10.1007/s10118-026-3738-y.

Yong-Li Du, Yong-Fan Cao, Zhen-Zhu Cao, et al. High Ionic Conductivity and Transfer Number of Composite Solid Electrolyte for Advanced Lithium Battery by Synergetic Effect of Halloysite Nanotube and High-entropy Zeolitic Imidazolate Frameworks[J]. Chinese Journal of Polymer Science, 2026, 44(10): 3513-3527. DOI： 10.1007/s10118-026-3738-y.

摘要

A flexible polyvinylidene fluoride (PVDF)-based composite solid electrolyte with 1D halloysite nanotubes (HNTs) and porous high-entropy zeolitic imidazolate framework (HE-ZIF) was prepared

achieving high ionic conductivity

transference number and dendrite suppression.

Abstract

Composite solid-state electrolytes (CSEs) with excellent flexibility and high safety hold great potential for high performance lithium batteries. However

its low room temperature ionic conductivity and transfer number have plagued its practical application. In this work

local Li diffusion was tailored by the synergetic effect of halloysite nanotubes (HNTs) and high-entropy ZIF in a polyvinylidene fluoride/LITFSI/Li

6.85

2.95

0.05

1.85

0.15

matrix. The anchoring of TFSI

–

anions by the rich open metal sites in HE-ZIF and the inner positively wall in HNT

combined with the continuous diffusion pathway of Li

built by the negatively surface of HNT

distinctly enhances the ionic conductivity and transfer number of the electrolyte. A high ionic conductivity (1.06×10

–3

S·cm

–1

at 30 °C) and high Li

transference number (0.86) were achieved in PLLH-HE. The lithium symmetric battery (Li//PLLH-HE//Li) exhibited excellent interfacial compatibility and a high critical current density (CCD

2.38 mA·cm

–2

). A lithium metal battery assembled with LiFePO

(LFP) cathodes exhibited a high discharge specific capacity of 141 mAh·g

–1

after 400 cycles at 0.5 C

while the cell assembled with LiNi

0.8

0.1

(NCM811) also delivered a high discharge specific capacity of 140.1 mAh·g

–1

at 1 C after 600 cycles. This work reveals the critical role of local Li diffusion and provides a general method for enhancing the electrochemical properties of CSEs for solid state batteries.

关键词

Keywords

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