First-Principles Simulations of Heterogeneous Interfaces for the Water-Energy Nexus*

Understanding physicochemical processes at heterogeneous interfaces is critical in a wide range of emerging technologies, from energy storage and conversion to water treatment. In this talk, I will review our recent activities in the simulation of electrochemical interfaces using first-principles approaches. I will discuss how first-principles simulations have been applied to elucidate chemical evolutions and degradation mechanism of materials at the interface with aqueous electrolytes. In addition, I will show how first-principles calculations have been combined with implicit solvation models to understand electric double layer effects in porous materials. Finally, I will discuss how first-principles simulations are combined with multi modal characterization techniques to provide mechanistic understandings of ion transport and selectivity in sub-nm nanopores. Our results demonstrate the complex synergy between interfacial chemistry, solvation effects and applied potentials, leading to behavior that qualitatively deviates from conventional models.