Modulating Interfacial Solvation via Ion Dipole Interactions for Low-Temperature and High-Voltage Lithium Batteries.

Angew Chem Int Ed Engl

State Key Laboratory of Advanced Chemical Power Sources, Engineering Center on High-efficiency Energy Storage (Ministry of Education), Key Laboratory of Advanced Energy Materials (Ministry of Education), Frontiers Science Center for New Organic Matter (Ministry of Education), College of Chemistry, N

Published: January 2025


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Article Abstract

Extending the stability of ether solvents is pivotal for developing low-temperature and high-voltage lithium batteries. Herein, we elucidate the oxidation behavior of tetrahydrofuran with ternary BF , PF and difluoro (oxalato) borate anions and the evolution of interfacial solvation environment. Combined in situ analyses and computations illustrate that the ion dipole interactions and the subsequent formation of ether-Li-anion complexes in electrolyte rearrange the oxidation order of solvated species, which enhances the electrochemical stability of ether solvent. Furthermore, preferential absorption of anions on the surface of high-voltage cathode favors the formation of a solvent-deficient electric double layer and an anti-oxidation cathode electrolyte interphase, inhibiting the decomposition of tetrahydrofuran. Remarkably, the formulated electrolyte based on ternary anion and tetrahydrofuran solvent endows the LiNiCoMnO cathode with considerable rate capability of 5.0 C and high capacity retention of 93.12 % after 200 cycles. At a charging voltage of 4.5 V, the Li||LiNiCoMnO cells deliver Coulombic efficiency above 99 % at both 25 and -30 °C.

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http://dx.doi.org/10.1002/anie.202415853DOI Listing

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