DFT simulations of lean NOx catalysis

I&EC 125

Ye Xu, xuy2@ornl.gov1, William F. Schneider, wschneider@nd.edu2, and Rachel B. Getman, rgetman@nd.edu2. (1) Center for Nanophase Materials Sciences and Chemical Sciences Division, Oak Ridge National Laboratory, P.O. Box 2008, MS-6494, Oak Ridge, TN 37831-6494, (2) Department of Chemical and Biomolecular Engineering, University of Notre Dame, 182 Fitzpatrick Hall, Notre Dame, IN 46556
NOx (x = 1, 2) emissions control is one of the key unresolved environmental issues in the clean combustion of fossil fuels. Various catalytic strategies exist to promote the reduction of NOx to N2, and most of these depend in part on the catalytic oxidation of NO to NO2. In this work, we apply density functional theory methods to explore NO catalytic oxidation on model Pt materials. We consider the nature and stability of surface-bound reactants, products, and possible intermediates over a range of coverage conditions on a Pt(111) surface. We show that, because of the weak reducing power of NO, catalytic oxidation is highly sensitive to the oxygen coverage of the surface and must compete with strongly bound NOx surface intermediates. We also explore the extensions of these ideas to few atom clusters of Pt, where the ability to adsorb oxygen becomes a strong funciton of particle size.
 

Computational Material Design in Chemical Industries, Sponsored by Novel Chemistry with Industrial Applications Sub-Division
8:30 AM-11:40 AM, Tuesday, 12 September 2006 Moscone Center -- Room 252/254, Oral

Division of Industrial & Engineering Chemistry

The 232nd ACS National Meeting, San Francisco, CA, September 10-14, 2006