(2dr) Mulitscale Modeling of Interfacial Electrocatalytic Processes

Electrochemical processes are expected to play a central role in the transition to net-zero carbon emissions and help address the looming climate crisis. The complex nature of the electrode-electrolyte interface involving interactions across different time- and length-scales makes it extremely challenging to understand electrochemical processes. Rapid advancements in computational methods and high-performance computing in the recent years have enabled simulations to provide unprecedented insights into the atomistic structure of the reaction environment, elucidating reaction mechanisms and guiding catalyst design. However, a number of challenges still remain.These challenges include: (i) understanding the atomistic structure of the electrode-electrolyte interface under operando conditions, (ii) Estimating electrochemical reaction kinetics that are important to understand reaction pathways and predict product selectivity in multi-step electrocatalytic reactions and (iii) Incorporating the effects of various components of the electrolyte environment including mass transport, double-layer charging and solution phase reactions in modeling studies. Accounting for all these aspects necessitates the development of a multiscale approach to understand and predict electrochemical processes for energy conversion.

In my previous research, we have addressed different aspects of the aforementioned challenges using a combination of simulation techniques including density functional theory based molecular dynamics (DFT-MD), ab-initio microkinetic simulations and continuum transport modeling. For instance, we used DFT-MD simulations of metal-water interfaces to understand their structure, estimate solvation energies and identify trends in the potential of zero charge.[1,2] We identify simple descriptors to predict these quantities, thereby circumventing the need for expensive DFT-MD simulations. Using constant-potential DFT simulations (in combination with experiments), we elucidated reaction mechanisms of complex multi-step electrocatalytic reactions including electrochemical CO2 reduction [3,4] and electrochemical biomass conversion [5,6]. Furthermore, we have investigated mechanisms behind the effects of the reaction environment (i.e. electrolyte pH, cations and anions) on the activity and selectivity of several electrochemical processes. [7, 8]

I aim to develop an interdisciplinary research program to gain a fundamental understanding of interfacial electrocatalytic processes. The overarching goal of my research program is to be able to realize the full potential of electrocatalytic processes in the transition to net-zero carbon emissions.

Teaching and mentoring