Unveiling high-power and high-safety lithium-ion battery separator based on interlayer of ZIF-67/cellulose nanofiber with electrospun poly(vinyl alcohol)/melamine nonwoven membranes

Xiao-Wei Wu; Chelladurai Karuppiah; Yi-Shiuan Wu; Bo-Rong Zhang; Li-Fan Hsu; Jeng-Ywan Shih; Ying-Jeng James Li; Tai-Feng Hung; Sayee Kannan Ramaraj; Rajan Jose; Chun-Chen Yang

doi:10.1016/j.jcis.2023.12.098

Unveiling high-power and high-safety lithium-ion battery separator based on interlayer of ZIF-67/cellulose nanofiber with electrospun poly(vinyl alcohol)/melamine nonwoven membranes

J Colloid Interface Sci. 2024 Mar 15:658:699-713. doi: 10.1016/j.jcis.2023.12.098. Epub 2023 Dec 19.

Authors

Affiliations

¹ Battery Research Center of Green Energy, Ming Chi University of Technology, New Taipei City 24301, Taiwan, ROC; Department of Chemical Engineering, Ming Chi University of Technology, New Taipei City 243, Taiwan, ROC.
² Battery Research Center of Green Energy, Ming Chi University of Technology, New Taipei City 24301, Taiwan, ROC. Electronic address: kcdurai.rmd@gmail.com.
³ Battery Research Center of Green Energy, Ming Chi University of Technology, New Taipei City 24301, Taiwan, ROC.
⁴ PG and Research Department of Chemistry, Thiagarajar College, Madurai, Tamil Nadu, India.
⁵ Center for Advanced Intelligent Materials & Faculty of Industrial Sciences and Technology, University Malaysia Pahang Al-Sultan Abdullah, 26300 Kuantan, Pahang, Malaysia.
⁶ Battery Research Center of Green Energy, Ming Chi University of Technology, New Taipei City 24301, Taiwan, ROC; Department of Chemical Engineering, Ming Chi University of Technology, New Taipei City 243, Taiwan, ROC; Department of Chemical and Materials Engineering, Chang Gung University, Kwei-shan, Taoyuan 333, Taiwan, ROC. Electronic address: ccyang@mail.mcut.edu.tw.

PMID: 38141392
DOI: 10.1016/j.jcis.2023.12.098

Abstract

Due to the poor thermal stability of conventional separators, lithium-ion batteries require a suitable separator to maintain system safety for long-term cycling performance. It must have high porosity, superior electrolyte uptake ability, and good ion-conducting properties even at high temperatures. In this work, we demonstrate a novel composite membrane based on sandwiching of zeolitic imidazole frameworks-67 decorated cellulose acetate nanofibers (ZIF-67@CA) with electrospun poly(vinyl alcohol)/melamine (denoted as PVAM) nonwoven membranes. The as-prepared sandwich-type membranes are called PVAM/x%ZIF-67@CA/PVAM. The middle layer of composite membranes is primarily filled with different weight percentages of ZIF-67 nanoparticles (x = 5, 15, and 25 wt%), which both reduces the non-uniform porous structure of CA and increases its thermal stability. Therefore, our sandwich-type PVAM/x%ZIF-67@CA/PVAM membrane exhibits a higher thermal shrinkage effect at 200 °C than the commercial polyethylene (PE) separator. Due to its high electrolyte uptake (646.8%) and porosity (85.2%), PVAM/15%ZIF-67@CA/PVAM membrane achieved high ionic conductivity of 1.46 × 10^-3 S cm^-1 at 70 °C, as compared to the commercial PE separator (ca. 6.01 × 10^-4 S cm^-1 at 70 °C). Besides, the cell with PVAM/15%ZIF-67@CA/PVAM membrane shows an excellent discharge capacity of about 167.5 mAh g^-1after 100 cycles at a 1C rate with a capacity retention of 90.3%. The ZIF-67 fillers in our sandwich-type composite membrane strongly attract anions (PF₆^-) through Lewis' acid-base interaction, allowing uniform Li⁺ ion transport and suppressing Li dendrites. As a result, we found that the PVAM/15%ZIF-67@CA/PVAM composite nonwoven membrane is applicable to high-power, high-safety lithium-ion battery systems that can be used in electric vehicles (EVs).

Keywords: Cellulose nanofibers; Electrospinning; Metal-organic frameworks; Poly(vinyl alcohol); Separator modification; ZIF-67 nanoparticles.