Research

Summary

The electrochemical interface is a critical zone that enables chemical transformations and is arguably the most vital—yet least understood part of an electrochemical system. Our understanding of electrochemical interfaces remains in its infancy due to their inherent complexity and the limited experimental and computational tools currently available to investigate them. For computational tools to function as accurate microscopes of the electrified interface, it is essential to develop realistic models that can capture the diverse physicochemical phenomena occurring across a wide range of length and time scales.

The DELI Lab aims to leverage atomistic simulations (such as density functional theory, molecular dynamics, and enhanced sampling), accelerated by machine learning-based approaches, alongside mesoscale simulations (microkinetic modeling, kinetic Monte-Carlo) and transport modeling to advance our understanding of electrochemical interfaces. These insights will be used to design next-generation electrochemical interfaces for applications in energy storage and conversion.

Key subtopics and and modeling techniques

Research Directions

Electrocatalytic reactions in non-aqueous electrolytes

We are interested in developing design principles to utilize non-aqueous 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 currently working on understanding the molecular interactions that govern water organization and activity in blended (organic solvent/water) electrolytes its impact on proton-coupled electron transfer kinetics 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 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 the interface structure and dynamics, and the kinetics of elementary chemical and proton-coupled electron transfer steps.