Research

The ultimate goal of our research program is to establish a link between electronic structure of catalyst particles and actual catalytic performance. To this end we are developing a methodology to:

 

· determine the detailed electronic surface structure and its effect on surface microstructure,

 

· establish the nature of adsorbate-surface and adsorbate-adsorbate interactions,

 

· quantify the energetics of each elementary path and governing surface phenomena,

 

· simulate the myriad of competing mechanistic and pathways which compromise the measurable kinetics,

 

· predict process operating performance.

 

To achieve these research goals, we essentially tie tunable atomic structural levers to overall process chemistry. This provides a framework by which we can attempt to computationally manipulate microstructural variables (atomic promoters, selective poisons, etc.) in an effort to optimize desired product yields and properties.

Our approach can be described as a molecular reaction engineering analysis of complex catalytic systems, whereby we couple first-principle quantum chemical methods with stochastic modelling techniques to traverse the vastly different structural and reactivity hierarchical levels. Density functional methods are used to probe the detailed electronic structure and adsorbate-surface interactions of transition-metal-containing surfaces and particles. Energetics and kinetics for key elementary steps occurring on the catalytic surface (adsorption, desorption, diffusion, surface reactions, etc.) are also predicted from quantum chemical calculations. The global process chemistry (catalytic as well as thermal) is determined by robust simulation of complex networks of molecular-surface events and/or molecule-molecule interactions.

We are investigating various selective oxidation routes on transition metals, bi metallics and transition metal oxide particles to understand the active surface structure (both geometric and electronic), adsorbate binding energetics, and available surface reaction pathways. More specifically we are looking at:

 

· The oxidation of industrial production of monomer intermediates for Lycra,

 

· The synthesis of vinyl acetate monomers over palladium and palladium. acetate.

COMPUTATIONAL CATALYSIS GROUP

Department of Chemical Engineering. University of Virginia

Department of Chemical Engineering
University of Virginia
Charlottesville, VA 22904

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