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Solid-state batteries (SSBs) can offer a paradigm shift in battery safety andenergy density. Yet, the promise hinges on the ability to integratehigh-performance electrodes with state-of-the-art solid electrolytes. Forexample, lithium (Li) metal, the most energy-dense anode candidate, suffersfrom severe interfacial chemomechanical issues that lead to cell failure. Lialloys of In/Sn are attractive alternatives, but their exploration has mostlybeen limited to the low capacity(low Li content)and In rich Li$_x$In(x$\leq$0.5). Here, the fundamental electro-chemo-mechanical behavior of Li-Inand Li-Sn alloys of varied Li stoichiometries is unravelled in sulfideelectrolyte based SSBs. The intermetallic electrodes developed through acontrolled synthesis and fabrication technique display impressive(electro)chemical stability with Li$_6$PS$_5$Cl as the solid electrolyte andmaintain nearly perfect interfacial contact during the electrochemical Liinsertion/deinsertion under an optimal stack pressure. Their intriguingvariation in the Li migration barrier with composition and its influence on theobserved Li cycling overpotential is revealed through combined computationaland electrochemical studies. Stable interfacial chemomechanics of the alloysallow long-term dendrite free Li cycling (>1000 h) at relatively high currentdensities (1 mA cm$^{-2}$) and capacities (1 mAh cm$^{-2}$), as demonstratedfor Li$_{13}$In$_3$ and Li$_{17}$Sn$_4$, which are more desirable from acapacity and cost consideration compared to the low Li content analogues. Thepresented understanding can guide the development of high-capacity Li-In/Snalloy anodes for SSBs.

Favorable Interfacial Chemomechanics Enables Stable Cycling of High Li-Content Li-In/Sn Anodes in Sulfide Electrolyte Based Solid-State Batteries