Developing Multi-Scale Models for the Effective Design of Hydrothermally Stable Single-Site Catalysts for Low-Temperature CO Emissions Removal
EMSL Project ID
50480
Abstract
The research objective of this proposal is to develop a multi-scale model that will predict the catalytic behavior of low temperature single-atom exhaust catalysts in real-world conditions. The central hypothesis here is that the chemical modification of a first-row transition metal oxide with an atomically dispersed precious metal will display theoretical efficiencies that are superior to pure-precious-metal catalysts, and that these high efficiencies will be connected to the support's ability to control the oxidation state of the atomically dispersed metal. The expected contributions of this project are significant since it will lead to a comprehensive and predictive model toward the low-temperature elimination of CO, which will be experimentally validated by our collaborators. The proposed research will determine the electronic structure fingerprints that describe the synergetic properties between a single-site Pt atom and a copper oxide surface. The PI will determine such electronic fingerprints of the catalytically active Pt atom using density functional theory and predict how one can prevent its deactivation. The influence of the cooperative effects between a copper surface oxide and an isolated Pt atom on the oxidation kinetics under realistic reaction conditions will also be examined. From here, a multi-scale model using a combination of density functional theory calculations and kinetic Monte Carlo simulations capturing the essential features at the mesoscale, such as the influence of steam on the oxidation kinetics, will be developed. The complexity of the models that will be developed necessitates that we gain access to the Cascade cluster to do the corresponding DFT calculations.
Project Details
Start Date
2018-10-01
End Date
2019-09-30
Status
Closed
Released Data Link
Team
Principal Investigator
Team Members
Related Publications
Balema T.A., N.Z. Ulumuddin, C.J. Murphy, D.P. Slough, Z.C. Smith, R.T. Hannagan, and N.A. Wasio, et al. 2019. "Controlling Molecular Switching via Chemical Functionality: Ethyl vs Methoxy Rotors." Journal of Physical Chemistry C. doi:10.1021/acs.jpcc.9b06664
Larson A.M., K.J. Groden, R.T. Hannagan, J. McEwen, and E.H. Sykes. 2019. "Understanding Enantioselective Interactions by Pulling Apart Molecular Rotor Complexes." ACS Nano 13, no. 5:5939-5946. doi:10.1021/acsnano.9b01781
Therrien A.J., A.J. Hensley, R.T. Hannagan, A.C. Schilling, M.D. Marcinkowski, A.M. Larson, and J. McEwen, et al. 2019. "Surface-Templated Assembly of Molecular Methanol on the Thin Film “29” Cu(111) Surface Oxide." Journal of Physical Chemistry C 123, no. 5:2911–2921. doi:10.1021/acs.jpcc.8b10284