(Invited) Computational Design and Analysis of Novel Battery Electrolytes Driven by the Grotthuss Mechanism

Candidate systems for next-generation electrolyte materials, such as deep eutectic solvents and ionic liquids, often suffer from high viscosities, which suppresses rates of charge transport and limits their performance characteristics. A strategy for circumventing this problem is to leverage the structural or Grotthuss mechanism of proton transport through hydrogen-bond networks, which can exhibit high proton diffusion rates even when rates of vehicular charge transport are poor. In this talk, I will describe a project aimed at leveraging computational design and simulation approaches, in combination with experimental synthesis and characterization, to develop a novel class of battery electrolytes based on the structural/Grotthuss diffusion mechanism. The workflow involves identification of a suitable proton-carrier liquid, a proton source, and a redox-active species capable of undergoing proton-coupled electron transfer (PCET) reactions. I will discuss the computational methods, which involve a combination of machine learning and first-principles simulation techniques, candidate chemical species for each of the components, first simulation and experimental protocols for combining these components into a high-performance electrolyte, preliminary results, and next steps in the evolution of the project. This work will serve to illustrate both the power of modern computational approaches in the design of electrochemical systems but also to broaden the perspective on what constitutes a “breakthrough” electrolyte.