Lithium-Rich Porous Aromatic Framework-Based Quasi-Solid Polymer Electrolyte for High-Performance Lithium Ion Batteries

Zhangnan Li; Liying Wang; Mengxuan Yu; Yuhan Liu; Baijun Liu; Zhaoyan Sun; Wei Hu; Guangshan Zhu

doi:10.1021/acsami.2c15810

Lithium-Rich Porous Aromatic Framework-Based Quasi-Solid Polymer Electrolyte for High-Performance Lithium Ion Batteries

ACS Appl Mater Interfaces. 2022 Dec 7;14(48):53798-53807. doi: 10.1021/acsami.2c15810. Epub 2022 Nov 28.

Authors

Zhangnan Li¹, Liying Wang¹, Mengxuan Yu¹, Yuhan Liu¹, Baijun Liu², Zhaoyan Sun³, Wei Hu¹, Guangshan Zhu¹

Affiliations

¹ Faculty of Chemistry, Northeast Normal University, 5268 Renmin Street, Changchun, Jilin130024, P. R. China.
² Faculty of Chemistry, Jilin University, 2699 Qianjin Street, Changchun130012, P. R. China.
³ State Key Laboratory of Polymer Physics and Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, 5625 Renmin Street, Changchun130022, P. R. China.

PMID: 36441518
DOI: 10.1021/acsami.2c15810

Abstract

The development of solid polymer electrolytes (SPEs) with high ionic conductivity, wide electrochemical window, and high mechanical strength is the key factor to realize high-energy-density solid lithium ion batteries (SLIBs). Porous aromatic frameworks (PAFs) have the advantages of high porosity, easily functionalized molecular structure, and rigid stable framework, which fully meet the requirements of solid polymer electrolytes with high Li⁺ capacity, fast Li⁺ transport, and safety. Herein, a lithium-rich amidoxime (AO)-modified porous aromatic framework (PAF-170-AO) was obtained through the absorption of LiTFSI by amidoxime groups and abundant pores and then compounded with poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) to prepare a PAF-based quasi-solid polymer electrolyte (PAF-QSPE) with only tiny amounts of plasticizer (∼12 μL). The amidoxime groups of PAF-170-AO restricted the movement of the anions of LiTFSI through hydrogen bonding, which effectively promoted the dissociation and migration number of Li⁺ (t_Li⁺), reduced the concentration polarization, and inhibited the growth of lithium dendrites. The PAF-QSPE exhibited a high ionic conductivity of 1.75 × 10^-4 S cm^-1 and t_Li⁺ of 0.55 at room temperature. The activation energy was as low as 0.136 eV. Furthermore, the assembled SLIBs with the PAF-QSPE presented a discharge capacity of 163 mAh g^-1 at 0.2 C and a capacity retention rate of 96% after 350 cycles, illustrating a stable cycling performance. This work demonstrated the great application potential of lithium-rich PAFs in QSPEs.

Keywords: LiTFSI; hydrogen bond; porous aromatic frameworks; quasi-solid polymer electrolyte; solid lithium ion batteries.