Research
Summary
The electrochemical interface is a critical zone where chemical transformations occur and is arguably the most vital, yet least understood part of an electrochemical system. Our understanding of these interfaces remains limited because of their inherent complexity and the paucity of experimental and computational tools available to probe them under reaction conditions. For computational methods to serve as accurate microscopes of the electrified interface, realistic models are needed that capture the diverse physicochemical phenomena spanning experimentally relevant length and time scales.
The DELI Lab seeks to understand how operating conditions determine the physical and chemical state of electrochemical interfaces, and how this evolving state controls reactivity. We combine first-principles methods, machine-learning accelerated molecular dynamics, statistical thermodynamics, and kinetic modeling to connect electrolyte composition, interfacial structure, reaction kinetics, and catalyst restructuring. A parallel focus is the development and validation of computational frameworks that describe these interfaces faithfully across experimentally relevant length and time scales.
Modeling techniques
Research Directions
Electrocatalytic reactions in complex electrolytes
We are interested in developing design principles to utilize non-aqueous and water-in-salt (WiS) electrolytes in a variety of electrochemical transformations. This is of interest given the vast design space - both in terms of the organic solvent and the proton donor compared to aqueous electrolytes. We are interested in understanding the molecular interactions that govern water organization and activity in blended (organic solvent/water) and WiS electrolytes, and their impact on proton-coupled electron transfer kinetics for reactions such as hydrogen evolution and CO reduction at electrified interfaces.
Electrode dissolution and restructuring under operando conditions
Electrocatalysts are highly dynamic under operando conditions and often undergo significant restructuring that impacts their stability and reactivity. Dissolution based pathways are a major contributor in this regard, and can be influenced by a number of factors including surface coordination, adsorbates, ions, pH, applied potential etc. We are interested in understanding the mechanisms that drive dissolution and the associated restructuring of (electro)catalysts under reaction conditions, and their implications on catalytic activity and stability.
Temperature effects in electrocatalysis
Electrocatalytic reactions are often studied at room temperature, despite commercial applications often requiring elevated temperatures for optimal performance. Recently, temperature has also been shown to provide insights into key properties such as entropy, interfacial structure and their impact on electrochemical kinetics. We are interested in developing a molecular level understanding of how temperature impacts bulk and interface structure, dynamics, and the kinetics of elementary chemical and proton-coupled electron transfer steps.
We acknowledge funding and HPC support from the following organizations
