Gu Mengjia, Zhou Xunzhu, Yang Qian, Chu Shenxu, Li Lin, Li Jiaxin, Zhao Yuqing, Hu Xing, Shi Shuo, Chen Zhuo, Zhang Yu, Chou Shulei, Lei Kaixiang
Tianjin Key Laboratory of Materials Laminating Fabrication and Interface Control Technology, School of Materials Science and Engineering, Hebei University of Technology, Tianjin, 300401, China.
Institute for Carbon Neutralization Technology, College of Chemistry and Materials Engineering, Wenzhou University, Wenzhou, Zhejiang, 325035, China.
Angew Chem Int Ed Engl. 2024 Jul 22;63(30):e202402946. doi: 10.1002/anie.202402946. Epub 2024 Jun 19.
Electrolytes with anion-dominated solvation are promising candidates to achieve dendrite-free and high-voltage potassium metal batteries. However, it's challenging to form anion-reinforced solvates at low salt concentrations. Herein, we construct an anion-reinforced solvation structure at a moderate concentration of 1.5 M with weakly coordinated cosolvent ethylene glycol dibutyl ether. The unique solvation structure accelerates the desolvation of K, strengthens the oxidative stability to 4.94 V and facilitates the formation of inorganic-rich and stable electrode-electrolyte interface. These enable stable plating/stripping of K metal anode over 2200 h, high capacity retention of 83.0 % after 150 cycles with a high cut-off voltage of 4.5 V in KMnO//K cells, and even 91.5 % after 30 cycles under 4.7 V. This work provides insight into weakly coordinated cosolvent and opens new avenues for designing ether-based high-voltage electrolytes.
具有阴离子主导溶剂化作用的电解质是实现无枝晶和高压钾金属电池的有前景的候选材料。然而,在低盐浓度下形成阴离子增强溶剂化物具有挑战性。在此,我们用弱配位共溶剂乙二醇二丁醚在1.5 M的中等浓度下构建了一种阴离子增强溶剂化结构。独特的溶剂化结构加速了钾的去溶剂化,将氧化稳定性增强至4.94 V,并促进了富含无机成分且稳定的电极-电解质界面的形成。这些使得钾金属阳极能够在2200小时以上稳定地进行电镀/剥离,在KMnO//K电池中,在4.5 V的高截止电压下循环150次后容量保持率为83.0%,在4.7 V下循环30次后甚至可达91.5%。这项工作为弱配位共溶剂提供了见解,并为设计醚基高压电解质开辟了新途径。