The ever-growing demand for low-cost, high-energy density batteries in electric transportation, robotics, and grid storage has necessitated exploration of new electrochemistry beyond the conventional Li-ion technology. In this context, rechargeable metal-sulfur batteries (RMSBs) offer tremendous promise owing to high theoretical specific energy (~10 times Li-ion), natural abundance of materials, low-cost, and use of non-toxic components. Unfortunately, long-standing issues with polysulfide dissolution in electrolyte, flammability of electrolyte, high reactivity of the metal anodes, and dendrite proliferation have precluded development of safe RMSBs that can effectively compete with existing Li-ion technology. Most of these daunting issues hindering practical implementation of RMSBs stem from dearth of atomic-scale understanding of solvation chemistry, ion-transport, chemical reactions, and nucleation/growth of interphases at electrode/electrolyte interfaces. In this talk, I will demonstrate how a synergistic integration of machine learning, first-principles calculations, ab initio/classical reactive molecular dynamics simulations can pave the path towards advancing such understanding; and accelerate design of next-generation electrolytes for both conventional (liquid electrolyte) and emerging solid-state RMSBs. Specifically, I will highlight two representative examples on how accurate materials modeling enabled design of (a) low-cost molten-salt electrolytes that enable fast-charging Al-S batteries (200 C) while impairing dendrite growth owing to formation of catenated AlnCl3n+1– species, (b) argyrodite sulfide electrolytes that provide superionic conduction of monovalent Li+/Na+ ions and excellent electrochemical stability against Li/Na metal owing to their unique defect structure and ion-disorder. Finally, I will showcase how we leveraged supervised machine learning to develop a classical reactive force field (ReaxFF) for Li-P-S system, which can accurately capture ion-transport, structural evolution, chemical reactions, interfacial processes, and effects of applied electric field relevant to Li-S batteries. I will discuss these results in the context of accelerating design of novel solid-state electrolytes for long-lived, stable, and high-energy density RMSBs.

Computationally guided design of electrolytes for high-performance rechargeable metal-sulfur batteries

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