Catalysis Research Campaign: An Integrated Multi-Capability Approach for Analysis of Catalytic Systems
EMSL Project ID
42295
Abstract
In this research campaign, advanced capabilities within the Environmental Molecular Sciences Laboratory (EMSL) at the Pacific Northwest National Laboratory will be integrated for in-depth, molecular level studies of catalytic processes that occur on a range of oxide materials under controlled conditions of temperature, pressure, and input gas composition. Although specific problems in the broad field of catalysis spur novel questions, an integrated and multi-capability infrastructure for studying catalytic systems provides the greatest efficiency in the study of a wide range of problems. We propose a research campaign where unique nuclear magnetic resonance (NMR) capabilities, including both in situ and advanced ex situ ultra-high field NMR techniques, will be developed and deployed. High-level computational analyses at the molecular level will also be established and coupled with NMR measurements to both explain and predict the structure and dynamics of molecules involved in catalytic reactions on surfaces, as well as how the temporal evolution of surface sites affects catalytic activity and performance. Specific NMR capabilities that will be developed and extended include continuous flow (CF) magic-angle spinning (MAS) NMR and discrete magic-angel turning (DMAT) NMR for use as in situ methods where pressure, gas flow, and temperature can be well controlled; multiple-quantum MAS NMR for ex situ probing of the distribution and evolution as a function of temperature of catalytic sites on alumina surfaces; and cross-polarization Carr-Purcell Meiboom-Gill spin echo MAS NMR for enhanced signal sensitivity leading to the quantitative description of Si and Al atomic ordering on amorphous silica-alumina and crystalline zeolite catalyst surfaces. For computational modeling of the catalyst surface, the active centers, the bulk lattice structures and NMR calculations we propose to perform periodic DFT calculations using a suite of codes (NWChem, Quantum Espresso, VASP). These calculations will be complemented with finite cluster and suitable embedding models (as needed). We will also perform NMR (GIAO) calculations using suitable finite cluster and embedding models (with NWChem and ADF) constructed from the optimized structures obtained using the periodic calculations. This approach will allow us to compare and contrast the utility of these models and to determine the validity of assuming that the local environment around the nucleus (or catalytic active center) of interest is sufficient to accurately describe the shielding and electric field gradients. Both experimental and computational data obtained in these studies will be integrated into databases and available for use (and potential re-use) by EMSL scientists, external project members, and the general scientific community. This research campaign will leverage the on-going development of the myEMSL environment through coupling with ongoing cyberinfrastructure projects at Penn State University and elsewhere. Finally, as this research campaign progresses, additional EMSL capabilities including the newly acquired He ion microscope will be leveraged to provide unprecedented details for understanding catalytic mechanisms and factors influencing the catalytic performance of a range of advanced materials.
Project Details
Project type
Research Campaign
Start Date
2011-01-17
End Date
2012-11-06
Status
Closed
Released Data Link
Team
Principal Investigator
Team Members
Related Publications
Andersen A, SM Kathmann, MA Lilga, KO Albrecht, RT Hallen, and D Mei. 2014. "Effects of Potassium Doping on CO Hydrogenation Over MoS2 Catalysts: A First-Principles Investigation." Catalysis Communications 52:92-97. doi:10.1016/j.catcom.2014.02.011
ao F, ED Walter, EM Karp, JY Luo, RG Tonkyn, JH Kwak, J Szanyi, and CHF Peden. 2013. "Structure-Activity Relationships in NH3-SCR over Cu-SSZ-13 as Probed by Reaction Kinetics and EPR Studies." Journal of Catalysis 300(1):20-29. doi:10.1016/j.jcat.2012.12.020
Baer DR, MH Engelhard, GE Johnson, J Laskin, J Lai, KT Mueller, P Munusamy, S Thevuthasan, H Wang, NM Washton, AC Elder, BL Baisch, AS Karakoti, SVNT Kuchibhatla, and DW Moon. 2013. "Surface Characterization of Nanomaterials and Nanoparticles: important needs and challenging opportunities." Journal of Vacuum Science and Technology A--Vacuum, Surfaces and Films 31(5):Article No. 050820. doi:10.1116/1.4818423.
Mei D. 2013. "First-principles characterization of formate and carboxyl adsorption on the stoichiometric CeO2(111) and CeO2(110) surfaces." Journal of Energy Chemistry 22(3):524-532. doi:10.1016/S2095-4956(13)60069-8
Mei D, VMC Lebarbier, RJ Rousseau, VA Glezakou, KO Albrecht, L Kovarik, MD Flake, and RA Dagle. 2013. "Comparative Investigation of Benzene Steam Reforming over Spinel Supported Rh and Ir Catalysts." ACS Catalysis 3(6):1133-1143. doi:10.1021/cs4000427