Fundamental Mechanistic Studies of Catalytic Hydrogen Production and Utilization
EMSL Project ID
30209
Abstract
This project will apply a unique capability at PNNL for heterogeneous catalysis R&D employing isotopic transient kinetic analysis (ITKA) techniques with mass spectroscopic and in-situ transmission FTIR analyses. The apparatus will enable an in situ probe of adsorbed reactants/intermediates/products on catalyst surfaces, as well as measuring gas phase concentrations to elucidate reaction mechanisms and kinetic parameters. Crucial to this effort will be computational modeling on high performance computers of the elementary reaction kinetics (i.e., reactant adsorption, dissociation, diffusion and reaction, and product desorption). The resulting data will be interpreted and applied to develop microkinetic models for catalytic reactions of importance to the USs future energy, environment, and economic security. Particular attention will be given to reactions of interest to the Presidents hydrogen economy initiative (e.g., fuel reforming, water-gas shift chemistries, partial oxidation of CO under hydrogen-rich environments-PROX, methane activation chemistries, and additional systems as they develop).
Project Details
Project type
Large-Scale EMSL Research
Start Date
2008-08-22
End Date
2011-09-30
Status
Closed
Released Data Link
Team
Principal Investigator
Team Members
Related Publications
Dai Y, B Lim, Y Yang, CM Cobley, W Li, EC Cho, B Grayson, PT Fanson, CT Campbell, Y Sun, and Y Xia. 2010. "A Sinter-Resistant Catalytic System Based on Platinum Nanoparticles Supported on TiO2 Nanofibers and Covered by Porous Silica." Angewandte Chemie International Edition 49(44):8165 –8168. doi:10.1002/anie.201001839
Mei D, L Xu, and GA Henkelman. 2009. "Potential Energy Surface of Methanol Decomposition on Cu(110) ." Journal of Physical Chemistry C 113(11):4522-4537.
Yang Y, CA Mims, D Mei, CHF Peden, and CT Campbell. 2013. "Mechanistic Studies of Methanol Synthesis over Cu from CO/CO2/H2/H2O Mixtures: the Source of C in Methanol and the Role of Water." Journal of Catalysis 298:10-17. doi:10.1016/j.jcat.2012.10.028
Yang Y, CA Mims, RS Disselkamp, CHF Peden, and CT Campbell. 2009. "Simultaneous MS-IR Studies of Surface Formate Reactivity Under Methanol Synthesis Conditions on Cu/SiO2." Topics in Catalysis 52(10):1440-1447. doi:10.1007/s11244-009-9320-3
Yang Y, CA Mims, RS Disselkamp, CHF Peden, and CT Campbell. 2009. "Simultaneous MS-IR Studies of Surface Formate Reactivity Under Methanol Synthesis Conditions on Cu/SiO2." Topics in Catalysis 52(10):1440-1447. doi:10.1007/s11244-009-9320-3
Yang Y, CA Mims, RS Disselkamp, JH Kwak, CHF Peden, and CT Campbell. 2010. "(Non) formation of methanol by direct hydrogenation of formate on copper catalysts." Journal of Physical Chemistry C 114(40):17205-17211. doi:10.1021/jp104068k
Zhao Y, Y Yang, CA Mims, CHF Peden, J Li, and D Mei. 2011. "Insight into methanol synthesis from CO2 hydrogenation on Cu(111): Complex reaction network and the effects of H2O." Journal of Catalysis 281(2):199-211. doi:10.1016/j.jcat.2011.04.012