Ma Xuemei, Fu Hongwei, Shen Jingyi, Zhang Dianwei, Zhou Jiawan, Tong Chunyi, Rao Apparao M, Zhou Jiang, Fan Ling, Lu Bingan
School of Physics and Electronics, Hunan University, Changsha, 410082, P. R. China.
School of Biology, Hunan Province Key Laboratory of Plant Functional Genomics and Developmental Regulation, Hunan University, Changsha, 410082, China.
Angew Chem Int Ed Engl. 2023 Dec 4;62(49):e202312973. doi: 10.1002/anie.202312973. Epub 2023 Oct 31.
Ether-based electrolytes are promising for secondary batteries due to their good compatibility with alkali metal anodes and high ionic conductivity. However, they suffer from poor oxidative stability and high toxicity, leading to severe electrolyte decomposition at high voltage and biosafety/environmental concerns when electrolyte leakage occurs. Here, we report a green ether solvent through a rational design of carbon-chain regulation to elicit steric hindrance, such a structure significantly reducing the solvent's biotoxicity and tuning the solvation structure of electrolytes. Notably, our solvent design is versatile, and an anion-dominated solvation structure is favored, facilitating a stable interphase formation on both the anode and cathode in potassium-ion batteries. Remarkably, the green ether-based electrolyte demonstrates excellent compatibility with K metal and graphite anode and a 4.2 V high-voltage cathode (200 cycles with average Coulombic efficiency of 99.64 %). This work points to a promising path toward the molecular design of green ether-based electrolytes for practical high-voltage potassium-ion batteries and other rechargeable batteries.
基于醚的电解质因其与碱金属阳极具有良好的兼容性以及高离子导电性,在二次电池领域颇具前景。然而,它们存在氧化稳定性差和毒性高的问题,导致在高电压下电解质严重分解,并且在电解质泄漏时会引发生物安全/环境问题。在此,我们通过合理设计碳链调控以产生空间位阻,报道了一种绿色醚溶剂,这种结构显著降低了溶剂的生物毒性并调整了电解质的溶剂化结构。值得注意的是,我们的溶剂设计具有通用性,且有利于形成以阴离子为主导的溶剂化结构,有助于在钾离子电池的阳极和阴极上均形成稳定的界面相。引人注目的是,这种基于绿色醚的电解质与钾金属和石墨阳极具有出色的兼容性,并且与4.2 V的高压阴极兼容(200次循环,平均库仑效率为99.64%)。这项工作为实际的高压钾离子电池和其他可充电电池的绿色醚基电解质的分子设计指明了一条充满希望的道路。