Due to its high capacity, renewability and environmental protection, organic carbonyl electrode materials have great prospects in the field of high-performance lithium batteries. However, the high solubility of these materials in conventional electrolytes hinders their practical application, which leads to poor cycling stability and severe shuttle effects.
Figure 1Design strategyAcademician of Nankai University, Xie WeiweiA series of hydrofluoroethers (HFES) with weak electrostatic effects on organic carbonyl cathode materials have been developed to solve the dissolution problem and achieve high cycling stability of lithium batteries. Theoretical calculations show that the intermolecular interaction between HFES and the carbonyl compound -pyrene-4,5,9,10-tetraone (PTO) is much lower than that of the commonly used solvent 1,2-dimethoxyethane (DME), which is mainly due to the difference in electrostatic interaction. Raman spectroscopy showed that 1,1,1,3,3,3-hexafluoro-2-methoxypropane (HFE-4) was partially involved in solvation, so the ionic conductivity was the highest among different HFE-based electrolytes. In-situ ultraviolet-visible spectroscopy (UV-VIS) showed that the dissolution of PTO electrodes in the DME-based electrolyte was much more severe than in the HFE-4-based electrolyte during discharge and charging.
Figure 2Therefore, the capacity retention rate of PTO in the HFE-4-based electrolyte (78% after 1000 cycles) was significantly higher than that in the DME-based electrolyte (34% after 400 cycles) compared with the DME-based electrolyte through theoretical calculations and experimental studies. In addition, the HFE-4-based electrolyte can also be used in other organic carbonyl cathode materials, such as perene-3,4,9,10-tetracarboxylic acid dianhydride (PTCDA). Overall, this work highlights the promising application of HFEs in prolonging the cycle life of organic carbonyl electrodes.
Figure 3Dissolution behavior and electrochemical performance of PTO during discharge and charging, regulating electrostatic interaction between hydrofluoroethers and carbonyl cathodes, toward highly stable lithium organic batteries journal of the american chemical society 2023. doi: 10.1021/jacs.3c12358