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
czz03@imut.edu.cn (Z.Z.C.)
wly2004@imut.edu.cn (L.Y.W.)
收稿:2026-04-02,
录用:2026-05-05,
网络首发:2026-07-06,
纸质出版:2026-06
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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. https://doi.org/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/OL]. Chinese Journal of Polymer Science, 2026, 441-15.
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. https://doi.org/10.1007/s10118-026-3738-y DOI:
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/OL]. Chinese Journal of Polymer Science, 2026, 441-15. DOI: 10.1007/s10118-026-3738-y.
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
La
2.95
Yb
0.05
Zr
1.85
Ta
0.15
O
12
matrix. The anchori
ng 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
4
(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
Co
0.1
Mn
0.1
O
2
(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.
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