Mechanochemical Reversible Complexation Mediated Polymerization Enabled Synthesis of Fluorinated Polyacrylate Copolymers for Room Temperature Solid-State Lithium Batteries

IF 5.1 1区化学 Q1 POLYMER SCIENCE

Macromolecules Pub Date : 2025-03-13 DOI:10.1021/acs.macromol.4c0298310.1021/acs.macromol.4c02983

Ziye Ren, Pan Mei, Chenyu Wang, Du Chen, Li Zhang, Wei Zhang*, Zhao Wang* and Zhengbiao Zhang*,

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引用次数: 0

Abstract

Solid polymer electrolytes (SPEs) have garnered significant interest in the advancement of solid-state lithium batteries (SSBs) due to their excellent safety, processability, and lightweight features. Currently, there is an urgent demand for the green synthesis of high performance SPEs for applications in SSBs. In this study, we report a one-pot mechanochemical reversible complexation mediated polymerization (mechano-RCMP) approach to synthesize fluorinated polyacrylates under solventless conditions. The mechano-RCMP approach demonstrated an efficient controlled polymerization process with quantitative monomer conversion through force induced activation of the carbon–iodine bond. The chain extension experiments confirmed the high chain-end functional groups of the polymers. Further copolymerization of heptafluorobutyl acrylate (HFBA) with butyl acrylate (BA) and methoxy polyethylene glycol acrylate (mPEG) resulted in the formation of P(BA-co-HFBA-co-mPEG), which demonstrated high thermal stability and amorphous characteristics. This copolymer film exhibited a wide electrochemical window (upper cutoff voltage up to 5.4 V) and high Li⁺ conductivity (1.3 × 10^–4 S cm^–1 at 30 °C). SSBs fabricated with the P(BA-co-HFBA-co-mPEG) film showed good cycling performance, maintaining a capacity retention of 98% after 100 cycles at room temperature.

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来源期刊

Macromolecules 工程技术-高分子科学

CiteScore

9.30

自引率

16.40%

发文量

942

审稿时长

2 months

期刊介绍： Macromolecules publishes original, fundamental, and impactful research on all aspects of polymer science. Topics of interest include synthesis (e.g., controlled polymerizations, polymerization catalysis, post polymerization modification, new monomer structures and polymer architectures, and polymerization mechanisms/kinetics analysis); phase behavior, thermodynamics, dynamic, and ordering/disordering phenomena (e.g., self-assembly, gelation, crystallization, solution/melt/solid-state characteristics); structure and properties (e.g., mechanical and rheological properties, surface/interfacial characteristics, electronic and transport properties); new state of the art characterization (e.g., spectroscopy, scattering, microscopy, rheology), simulation (e.g., Monte Carlo, molecular dynamics, multi-scale/coarse-grained modeling), and theoretical methods. Renewable/sustainable polymers, polymer networks, responsive polymers, electro-, magneto- and opto-active macromolecules, inorganic polymers, charge-transporting polymers (ion-containing, semiconducting, and conducting), nanostructured polymers, and polymer composites are also of interest. Typical papers published in Macromolecules showcase important and innovative concepts, experimental methods/observations, and theoretical/computational approaches that demonstrate a fundamental advance in the understanding of polymers.