First Principles Investigations of Adsorbate-Metal Interactions: Quantum Monte Carlo and Ab Initio Molecular Dynamics Simulations

PI Name: 
Jeffrey Greeley
Purdue University
Allocation Program: 
Allocation Hours at ALCF: 
50 Million
Research Domain: 
Materials Science

The chemistry and physics of water near metal surfaces is central to a host of critical technological applications, ranging from metal corrosion to fuel cell electrocatalysis. Experimental studies of water-metal interactions, while providing very useful information about single molecule or monolayer water adsorption on metals, are restricted to low temperatures and provide no direct insights into how bulk water reorganizes itself near metal surfaces. Computational studies, on the other hand, are suited to understanding the molecular-level details of water adsorption on surfaces. This project will advance the theoretical accuracy of current state-of-the art simulation approaches. New Quantum Monte Carlo and ab-initio molecular dynamics-based approaches will be used to explore novel aspects of the interaction of molecules that are central to electrocatalytic reactions and fuel cell science, including water, carbon monoxide, and nitrogen-containing compounds, with transition metal surfaces. These results will improve theoretical understanding of water metal interactions and provide improved technology for prediction and development in the various technological applications related to water-metal interactions.