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Regulating the Solvation Structure of Electrolyte via Dual-Salt Combination for Stable Potassium Metal Batteries.

Jimin ParkGwangeon OhUn-Hyuck KimMuhammad Hilmy AlfaruqiXieyu XuYangyang LiuShizhao XiongAdi Tiara ZikriYang-Kook SunJaekook KimJang-Yeon Hwang
Published in: Advanced science (Weinheim, Baden-Wurttemberg, Germany) (2023)
Batteries using potassium metal (K-metal) anode are considered a new type of low-cost and high-energy storage device. However, the thermodynamic instability of the K-metal anode in organic electrolyte solutions causes uncontrolled dendritic growth and parasitic reactions, leading to rapid capacity loss and low Coulombic efficiency of K-metal batteries. Herein, an advanced electrolyte comprising 1 M potassium bis(fluorosulfonyl)imide (KFSI) + 0.05 M potassium hexafluorophosphate (KPF 6 ) dissolved in dimethoxyethane (DME) is introduced as a simple and effective strategy of regulated solvation chemistry, showing an enhanced interfacial stability of the K-metal anode. Incorporating 0.05 M KPF 6 into the 1 M KFSI in DME electrolyte solution decreases the number of solvent molecules surrounding the K ion and simultaneously leads to facile K + de-solvation. During the electrodeposition process, these unique features can lower the exchange current density between the electrolyte and K-metal anode, thereby improving the uniformity of K electrodeposition, as well as potentially suppressing dendritic growth. Even under a high current density of 4 mA cm -2 , the K-metal anode in 0.05 M KPF 6 -containing electrolyte ensures high areal capacity and an unprecedented lifespan with stable Coulombic efficiency in both symmetrical half-cells and full-cells employing a sulfurized polyacrylonitrile cathode.
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