Chen Jiangchun, Lan Hao, Wang Sicong, Liu Xinyu, Zhu Qiaonan, Zhang Xudong, Tang Mengyao, Dong Shuai, Yang Jie, Kurbanov Mirtemir, Guo Lin, Wang Hua
School of Chemistry, Key Laboratory of Bio-Inspired Smart Interfacial Science and Technology of Ministry of Education, Beihang University, Beijing 100191, China.
The Analysis & Testing Center, Beihang University, Beijing 100191, China.
J Am Chem Soc. 2025 Jan 22;147(3):2393-2402. doi: 10.1021/jacs.4c12126. Epub 2025 Jan 9.
Potassium (K)-based batteries hold great promise for cryogenic applications owing to the small Stokes radius and weak Lewis acidity of K. Nevertheless, energy-dense (>200 W h kg) K batteries under subzero conditions have seldom been reported. Here, an over 400 W h kg K battery is realized at -40 °C via an anode-free and dual-ion strategy, surpassing these state-of-the-art K batteries and even most Li/Na batteries at low temperatures (LTs). By introduction of a strongly associating salt as an additive to this anode-free K battery, an anion-derived solid electrolyte interphase can be established for a highly reversible, zero-excess K plating/stripping behavior on a bare current collector. Meanwhile, a binary solvent is rationally designed for lowering the cation desolvation energy barrier, which ensures comparably facile cation and desolvation-free anion kinetics in this dual-ion structure even at LTs. Consequently, the K||Al half-cell delivers a high Coulombic efficiency of 99.98% at -40 °C. By pairing with a high-energy cathode, a proof-of-concept anode-free K dual-ion battery (N/P = 0) is fabricated, delivering a record-high energy density of 407 W h kg with stable cycling of 183 cycles (80% capacity retention) at -40 °C. This work paves a way toward energy-dense batteries at extreme scenarios.
基于钾(K)的电池由于K的斯托克斯半径小和路易斯酸性弱,在低温应用中具有很大的潜力。然而,很少有关于在零下条件下能量密度大于200 W h kg的K电池的报道。在此,通过无阳极和双离子策略在-40°C下实现了超过400 W h kg的K电池,超过了这些先进的K电池,甚至在低温下超过了大多数锂/钠电池。通过向这种无阳极K电池中引入一种强缔合盐作为添加剂,可以建立一种源自阴离子的固体电解质界面,以在裸集流体上实现高度可逆、零过量的K电镀/剥离行为。同时,合理设计了一种二元溶剂以降低阳离子去溶剂化能垒,这确保了即使在低温下,在这种双离子结构中阳离子和无去溶剂化阴离子的动力学也相对容易。因此,K||Al半电池在-40°C下具有99.98%的高库仑效率。通过与高能量阴极配对,制造了一种概念验证的无阳极K双离子电池(N/P = 0),在-40°C下实现了创纪录的407 W h kg的高能量密度和183次循环的稳定循环(容量保持率80%)。这项工作为极端情况下的高能量密度电池铺平了道路。