Authors
Dongmin Park, Kyunam Lee, June Lee, Jisub Kim, Jihoon Oh, Insu Hwang, Sujin Kim, Inwoo Kim, Minkwan Kim, Ali Coskun, Jang Wook Choi
Published in
Angewandte Chemie (International ed. in English). Pages e1576222. Aug 29, 2026. Epub Aug 29, 2026.
Abstract
Electrolyte engineering based on solvent fluorination has proven effective for stabilizing lithium (Li) metal batteries by weakening the Li+-solvent interaction. However, the influence of fluorination on the chemical reactivity of an electrolyte toward Li metal remains poorly understood. Here, the effects of fluorination are systematically investigated by increasing the degree of fluorination (from 2 to 5 substituents) of the terminal alkyl moieties of the 1-ethoxy-2-methoxyethane (EME) and 1-(2-methoxyethoxy)propane (MEP) backbones (denoted F2EME, F4MEP, and F5MEP). Fluorination-induced corrosion deviates from that suggested by conventionally calculated lowest unoccupied molecular orbital (LUMO)-based rationales; instead, it is quantitatively described by the local pKa as a site-specific thermodynamic descriptor of the fluorination-induced electronic effect. Among the three derivatives, F4MEP is identified as the optimal solvent; it is sufficiently fluorinated to promote the formation of an anion-rich solvation structure for an inorganic-rich, protective Li metal interphase, yet it is not severely corrosive as it is not over-fluorinated. Consequently, an F4MEP-based 20 µm-Li||LiNi0.8Co0.1Mn0.1O2 (NCM811) full-cell retains 80% of its capacity over 368 cycles. This study establishes the local pKa as a descriptor for evaluating the solvent corrosiveness and highlights the necessity of optimizing the degree of fluorination for high-performance Li metal battery electrolytes.
PMID:
42667610
Bibliographic data and abstract were imported from PubMed on 30 Aug 2026.
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