NMR and Computational Studies of Chemical Transformations at Complex Interfaces
EMSL Project ID
19795
Abstract
Catalysis provides the means of controlling the rates at which chemical bonds are formed or broken and the yields of desired products over undesired ones. New computational and experimental approaches are enabling scientists to obtain detailed insights into the steps involved in chemical bond formation and how one can control the energetics of transforming the chemical bonds from a set of reactants to a desired set of products. The direct coupling of theory and experiment is an extremely strong combination and is needed to advance catalytic science and our understanding of how to tailor chemical transformations for maximum activity and selectivity. A detailed understanding of the mechanisms involved in a catalytic reaction requires that we identify the nature of the active sites and of reaction intermediates, and that we probe dynamic processes starting when reactants enter the reaction zone until final products elute from the system. We have been and are developing novel NMR methods complementary to other in-situ spectroscopic techniques in order to improve our understanding of catalytic processes through in-situ investigations of the catalyst, the reaction intermediates, and the required elementary steps. Novel in-situ NMR probes have been developed. In combination with the NMR methods, we have been using high level computational electronic structure approaches to predict NMR chemical shifts to help interpret the experimental data. We are requesting joint access to both the high field nmr capabilities and the high performance massively parallel computing facility in the EMSL to do this work. This work is focused on the EMSL science theme: Interfacial Phenomena. The proposal is for 3 years and we provide requests for facilities access per year.
Project Details
Project type
Large-Scale EMSL Research
Start Date
2006-08-08
End Date
2009-09-30
Status
Closed
Released Data Link
Team
Principal Investigator
Team Members
Related Publications
Herrera JE, JH Kwak, JZ Hu, Y Wang, and CHF Peden. 2008. "Effects of novel supports on the physical and catalytic properties of tungstophosphoric acid for alcohol dehydration reactions." Topics in Catalysis 49(3-4):259-267. doi:10.1007/s11244-008-9081-4
Hu JZ, JH Kwak, Y Wang, CHF Peden, H Zheng, D Ma, and X Bao. 2009. "Studies of the Active Sites for Methane Dehydroaromatization Using Ultrahigh-Field Solid-State Mo95 NMR Spectroscopy." Journal of Physical Chemistry C 113(7):2936-2942. doi:10.1021/jp8107914
Mei, D.; Ge, Q.; Kwak, J.H.; Kim, D.H.; Szanyi, J.; Peden, C.H.F. "Adsorption and Formation of BaO Overlayers on γ Al2O3 Surfaces." J. Phys. Chem. C 112 (2008) 18050 18060.
Mei, D.; Ge, Q.; Kwak, J.H.; Kim, D.H.; Verrier, C.; Szanyi, J.; Peden, C.H.F. "Characterization of Surface and Bulk Nitrates of γ-Al2O3?Supported Alkaline Earth Oxides using Density Functional Theory." Phys. Chem. Chem. Phys. 11 (2009) 3380-3389.
Mei, D.; Ge, Q.; Szanyi, J.; Peden, C.H.F. "A First-Principles Analysis of NOx Adsorption on Anhydrous γ-Al2O3 Surfaces." J. Phys. Chem. C 113 (2009) 7779-7789.
Zhai HJ, S Li, DA Dixon, and LS Wang. 2008. "Probing the Electronic and Structural Properties of Chromium Oxide Clusters (CrO3)n- and (CrO3)n (n=1-5): Photoelectron Spectroscopy and Density Functional Calculations." Journal of the American Chemical Society 130(15):5167-5177.
Zheng H, D Ma, X Bao, JZ Hu, JH Kwak, Y Wang, and CHF Peden. 2008. "Direct Observation of the Active Center for Methane Dehydroaromatization Using an Ultrahigh Field 95Mo NMR Spectroscopy." Journal of the American Chemical Society 130(12):3722-3723. doi:10.1021/ja7110916