Fluorinated Segments
Engineering with Strongly Electron
Withdrawing Effect in Quasi Solid State Electrolyte for Fast Charging
and High Voltage Lithium Metal Batteries
Polyether electrolytes (PE) suffer from strong Li+–ether oxygen coordination and poor high voltage oxidative stability. Herein, we use in situ copolymerization to covalently graft the strongly electron-withdrawing −CF3 groups onto the backbone, synthesizing FPME, which delocalizes electron density around ether oxygens. Unlike physical blending, this covalent approach ensures molecular uniformity of electron-withdrawing effects, creating a weak coordination microenvironment that reshapes Li+ solvation and expedites ion transport. The electrolyte achieves 1.30 mS cm–1 at 30 °C. The −CF3 groups prevent lone-pair electron loss from ether oxygens, suppressing cathode side reactions and enhancing oxidation resistance, with an electrochemical window of 5.63 V, which contributes to enhanced long-term cycling stability. LFP||Li cell retains 65% capacity after 1000 cycles at 10 C, while NCM811||Li cell achieves 71% after 500 cycles at 1 C. This strategy enables fast charging and high energy density for solid-state lithium-metal batteries.
Polyether electrolytes are promising for lithium (Li) metal batteries yet suffer from insufficient Li+ conductivity, low oxidative thresholds, and unstable electrolyte–electrode interphases under high-voltage and fast-charging conditions. Herein, inspired by a natural sponge’s water absorption and release, we develop...
Li-Fen Zhang, Song Duan, Bing-Sen Qin et al.· Journal of the American Chem...· 0 citations
The development of lithium-oxygen (Li-O2) batteries, which possess high theoretical energy density, has long been hindered by safety issues and parasitic reactions arising from conventional liquid electrolytes. Gel polymer electrolytes (GPEs) have emerged as a promising alternative to settle these issues; however, th...
Bing Gan, Zheng-Zhou Tao, Jia-Cheng Wu et al.· ACS Applied Energy Materials· 0 citations
The cobalt-free LiNi0.5Mn1.5O4 (LNMO) cathode exhibits severe interfacial instability when employed with carbonate-based electrolytes. Here, we introduce methyl(3,3,3-trifluoropropyl)diethoxysilane (MFS) as a nonsacrificial additive that creates a molecular “repulsion layer” on LNMO. MFS preferentially adsorbs onto t...
Jun Gan, Qing Yang, Jin-Yan Guo et al.· ACS Energy Letters· 0 citations
Conventional linear polyether electrolytes feature abundant ether-oxygen sites that dominate the primary Li+ solvation shell, limiting anion participation and undermining ion transport and high-voltage stability. A backbone-mediated coordination-environment reshaping strategy is proposed by incorporating diglycidyl 1,2...
Ya-Jie Hu, Jian-Xin Wang, Ting Li et al.· Angewandte Chemie· 1 citation
Lithium-rich layered oxides (LLOs) deliver high energy density via coupled cationic/anionic redox, but high-voltage oxygen activation generates radical-rich interfaces that accelerate electrolyte decomposition, surface reconstruction, and mechanical failure. Although polyimide serves as an oxidation-resistant interphas...
Cheng-Han Li, Juan Wang, Pei Zou et al.· Angewandte Chemie· 0 citations
Polymer-based solid-state electrolytes are promising for safe and high-energy batteries but are fundamentally constrained by low ionic conductivity and unstable electrode interfaces. Here, we propose a molecular-level design using Na3P as a dual-function nanofiller in poly(vinylidene fluoride) (PVDF) electrolytes. Th...
Chen Li, Yong-Biao Mu, Tong-Tong Deng et al.· Journal of the American Chem...· 0 citations
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