Optimizing lithium-silver alloy phases for enhanced energy density and electrochemical performance

Lithium (Li) metal batteries though with high energy density are still facing issues like Li dendrite growth, dead Li formation, and thick solid electrolyte interphase (SEI) formation, hindering their long-term stability. Recently, Li-Ag alloys have been reported to potentially address these challenges possibly due to their superior conductivity, lithiophilicity, and mechanical stability. In the pursuit of high-energy-density batteries, Li-Ag alloys typically employ a high Li content phase (γ1). In this study, we applied density functional theory (DFT) calculations to compare the thermodynamic stability, Li adsorption, and Li diffusion of Ag-rich Li-Ag alloy within the γ1 phase (AR-γ1), Ag-poor Li-Ag alloy within the γ1 phase (AP-γ1), and pure Li. AR-γ1 showed better thermodynamic stability and improved Li adsorption and diffusion properties compared to AP-γ1 and pure Li. Electrochemical tests further confirmed the advantages of AR-γ1 in terms of electrode kinetics and cell stability compared to AP-γ1 and pure Li. Our study offers guidance for the selection of the most suitable Li-Ag alloys that can be utilized in high-energy-density lithium batteries.