(6an) Realistic and Affordable Ab Initio Calculations for Electrochemistry

Electrocatalysis currently plays a significant role in the world economy, and it holds tremendous promise to help meet future needs in areas including energy materials development and energy storage/conversion.  However, even the most basic electrochemical processes are incompletely understood.  To realize the full potential of electrocatalytic reactions, the fundamental reaction processes must be better characterized.  My previous work uniquely positions me to develop and utilize new modeling techniques that describe the nonidealities of surfaces and fluids, to re-evaluate the reaction mechanisms occurring in real electrochemical experiments.  In the poster session I will present my previous work, along with my recent findings in these areas.

My Ph.D. thesis explored different approaches to partitioning a molecular system from its environment, using both established and newly developed computational techniques.  Computational methods can easily become prohibitively expensive, especially when they are utilized to describe large and complex systems.  Choosing or developing the appropriate level of theory to describe the phenomenon of interest allows for better comparison against experiment.  I developed a new method for efficiently computing the dielectric properties of a molecular system from its component molecules, and tested it for ice and solid benzene.  The method successfully approximated the dielectric properties of ice at considerably reduced computational cost.  I also developed a framework for integrating new solvation models into highly accurate electronic structure methods, and I am a contributor to the open-source electronic structure code, JDFTx.  I have applied these methods and others to explore the optical properties of pentacene defects and to evaluate the properties of surfaces, ions, and molecules important for lithium sulfur batteries.

My postdoctoral research focuses on applying solvation methods to electrochemical systems to develop a deeper understanding of fundamental reaction processes.  I proposed a new mechanism for formic acid oxidation on Pt(111) under electrocatalytic conditions, in which I provide evidence that formate is the reactant, rather than the previously accepted formic acid.  This mechanism provides a new explanation for both the experimentally observed surface species and the lack of experimental evidence for other surface-bound species.  I also am currently developing a better understanding of the relationship between underpotential deposition of hydrogen and the hydrogen oxidation/evolution reactions on noble metals. 

Leveraging my understanding of the theoretical underpinning of electrochemical modeling, my future research will target challenges in electrochemical metal deposition and electrocatalysis for fuel production and consumption.