Low Melting Temperature Gallium-Indium Liquid Metal Anode for Solid-State Li-Ion Batteries

Solid-state Li-ion batteries are attracting attention for their enhanced safety features, higher energy density, and broader operational temperature range compared to systems based on liquid electrolytes. However, current solid-state Li-ion batteries face performance challenges, such as suboptimal cycling and poor rate capabilities, often due to inadequate interfacial contact between the solid electrolyte and electrodes. To address this issue, we incorporated a gallium-indium (Ga-In) liquid metal as the anode in a solid-state Li-ion battery setup, employing Li₆PS₅Cl as the solid electrolyte. Operating at room temperature, this configuration achieved an initial capacity of 389 mAh g^-1 and maintained 88% of this capacity after 30 cycles at a 0.05 C rate. It also demonstrated a capacity retention of 66% after 500 cycles at a 0.5 C rate. In comparison to solid anode materials, such as tin, the Ga-In liquid metal exhibited superior cycling stability and rate capacity, which is due to the self-healing and fluid properties of the alloy that ensure stable interfacial contact with solid electrolytes. In situ X-ray diffraction (XRD) and ex situ scanning electron microscope (SEM) analyses revealed that indium does not directly participate in the lithiation/delithiation process. Instead, it helps maintain the alloy's low melting point, facilitating its return to a liquid state after delithiation. In a comparative analysis of stack pressure during cycling in cells utilizing Ga-In liquid metal and tin, the Ga-In liquid metal cell demonstrated an ability to buffer pressure increases associated with deformation. These findings suggest a promising approach for enhancing solid-state batteries by integrating liquid metal anodes, which improve interfacial contact and stability.