Novel Quasi-Liquid K-Na Alloy as a Promising Dendrite-Free Anode for Rechargeable Potassium Metal Batteries

Abstract

Rechargeable potassium metal batteries are promising energy storage devices with potentially high energy density and markedly low cost. However, eliminating dendrite growth and achieving a stable electrode/electrolyte interface are the key challenges to tackle. Herein, a novel “quasi-liquid” potassium-sodium alloy (KNA) anode comprising only 3.5 wt% sodium (KNA-3.5) is reported, which exhibits outstanding electrochemical performance able to be reversibly cycled at 4 mA cm–2 for 2000 h. Moreover, it is demonstrated that adding a small amount of sodium hexafluorophosphate (NaPF6) into the potassium bis(fluorosulfonyl)imide electrolyte allows for the formation of the “quasi-liquid” KNA on electrode surface. Comprehensive experimental studies reveal the formation of an unusual metastable KNa2 phase during plating, which is believed to facilitate simultaneous nucleation and suppress the growth of dendrites, thereby improving the electrode's cycle lifetime. The “quasi-liquid” KNA-3.5 anode demonstrates markedly enhanced electrochemical performance in a full cell when pairing with Prussian blue analogs or sodium rhodizonate dibasic as the cathode material, compared to the pristine potassium anode. Importantly, unlike the liquid KNA reported before, the “quasi-liquid” KNA-3.5 exhibits good processability and can be readily shaped into sheet electrodes, showing substantial promise as a dendrite-free anode in rechargeable potassium metal batteries.