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Organic carbonyl electrode materials have shown great promise for high-performance lithium batteries due to their high capacity, renewability, and environmental friendliness. However, their practical application is hindered by the high solubility of these materials in traditional electrolytes, leading to poor cycling stability and serious shuttle effects. Here, we develop a series of hydrofluoroethers (HFEs) with weak electrostatic interaction toward organic carbonyl cathode materials, aiming to address the dissolution issue and achieve high cycling stability in lithium batteries. Theoretical calculations reveal that the electrostatic interactions between HFEs and pyrene-4,5,9,10-tetraone (PTO) are significantly weaker compared with common solvents such as 1,2-dimethoxyethane. Consequently, the dissolution of PTO in the HFE-based electrolyte is remarkably reduced, as observed by in situ ultraviolet-visible spectra. Notably, when using the electrolyte based on 1,1,1,3,3,3-hexafluoro-2-methoxypropane with a certain coordination ability, PTO exhibits excellent cycling stability with a high capacity retention of 78% after 1000 cycles. This work proposes the regulation of electrostatic interactions to inhibit the dissolution of organic carbonyl cathode materials and significantly enhance their cycle life.
Lü et al. (Thu,) studied this question.