MoCl<sub>5</sub>-mediated dual-track regulation unlocks high-voltage ether-based quasi-solid-state electrolytes.
basic_science · Level V
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- Record sourced from PubMed, PMID 42490431.
- Also identified by DOI 10.1126/sciadv.aeg9860.
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Abstract
In situ-polymerized 1,3-dioxolane (DOL) electrolytes offer a promising route to quasi-solid-state lithium metal batteries (QSSLMBs), yet their limited oxidative tolerance and unstable electrode interfaces restrict high-voltage operation. Here, a simulation-guided dual-track regulation strategy uses MoCl<sub>5</sub> as a multifunctional initiator to couple DOL ring-opening polymerization with Li-salt dissociation and inorganic interphase construction. MoCl<sub>5</sub> promotes formation of a high-molecular-weight poly(1,3-dioxolane) (PDOL) matrix and LiF/LiCl/Li<i><sub>x</sub></i>Mo<i><sub>y</sub></i>-enriched solid electrolyte interphase (SEI) and cathode electrolyte interphase (CEI), improving bulk stability, Li<sup>+</sup> transport, and interfacial robustness. The resulting MoCl<sub>5</sub>-regulated PDOL electrolyte achieves a Li<sup>+</sup> transference number of 0.71 and an electrochemical stability window of 4.7 V. Li||Li symmetric cells cycle for over 1000 hours at 5 mA cm<sup>-2</sup>, while high-voltage Li||LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub> (NCM811) cells retain over 95% capacity after 50 cycles at 2 C. This work establishes a design principle for multifunctional initiators and unlocks the high-voltage potential of ether-based electrolytes, advancing the practical application of QSSLMBs.