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High-Entropy Polymer Electrolytes Derived from Multivalent Polymeric Ligands for Solid-State Lithium Metal Batteries with Accelerated Li$^+$ Transport

Ye, Fangmin; Wang, Zhixin; Li, Mengcheng; Zhang, Jing; Wang, Dong; Liu, Meinan; Liu, Aiping; Lin, Hongzhen; Kim, Hee-Tak; Wang, Jian 1
1 Helmholtz-Institut Ulm (HIU), Karlsruher Institut für Technologie (KIT)

Abstract:

Solid-state polymer-based electrolytes (SSPEs) exhibit great possibilities in realizing high-energy-density solid-state lithium metal batteries (SSLMBs). However, current SSPEs suffer from low ionic conductivity and unsatisfactory interfacial compatibility with metallic Li because of the high crystallinity of polymers and sluggish Li$^+$ movement in SSPEs. Herein, differing from common strategies of copolymerization, a new strategy of constructing a high-entropy SSPE from multivariant polymeric ligands is proposed. As a protocol, poly(vinylidene fluoride-co-hexafluoropropylene) (PH) chains are grafted to the demoed polyethylene imine (PEI) with abundant −NH$_2$ groups via a click-like reaction (HE-PEIgPHE). Compared to a PH-based SSPE, our HE-PEIgPHE shows a higher modulus (6.75 vs 5.18 MPa), a higher ionic conductivity (2.14 × 10$^{–4}$ vs 1.03 × 10$^{–4}$ S cm$^{–1}$), and a higher Li$^+$ transference number (0.55 vs 0.42). A Li|HE-PEIgPHE|Li cell exhibits a long lifetime (1500 h), and a Li|HE-PEIgPHE|LiFePO$_4$ cell delivers an initial capacity of 160 mAh g$^{–1}$ and a capacity retention of 98.7%, demonstrating the potential of our HE-PEIgPHE for the SSLMBs.


Originalveröffentlichung
DOI: 10.1021/acs.nanolett.4c00154
Scopus
Zitationen: 3
Dimensions
Zitationen: 3
Zugehörige Institution(en) am KIT Helmholtz-Institut Ulm (HIU)
Publikationstyp Zeitschriftenaufsatz
Publikationsjahr 2024
Sprache Englisch
Identifikator ISSN: 1530-6984, 1530-6992
KITopen-ID: 1000171061
HGF-Programm 38.02.01 (POF IV, LK 01) Fundamentals and Materials
Erschienen in Nano Letters
Verlag American Chemical Society (ACS)
Band 24
Heft 23
Seiten 6850–6857
Vorab online veröffentlicht am 09.05.2024
Schlagwörter Solid polymer electrolyte, Li metal batteries, high-entropy polymer, polymeric ligand, Li+ transport
Nachgewiesen in Dimensions
Web of Science
Scopus
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