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Computational and Experimental Investigations into Ethanol and Higher (C2+) Oxygenate Synthesis from Biomass-derived Syngas Using Rh-based Catalysts


EMSL Project ID
47652

Abstract

Novel catalyst design is essential and combined experimental and theoretical/computational catalysis can provide the essential mechanisms, influence of promoters, energetics, selectivity, and activity for key reactions in the thermoconversion process. Reaction pathways calculated using quantum chemistry (using CP2K[1]) provide the reaction barriers used in microkinetic simulations to fundamentally understand and control catalyst design. Furthermore, experimental characterization using X-ray Photoelectron Spectroscopy (XPS), X-ray diffraction (XRD), and Transmission Electron Microscopy (TEM), provide chemical, structural, and morphological insight, validation, and closure for the computational studies. Enabled by the experimental characterization within the EMSL, this can become a powerful computational tool to screen various Rh-based (or other metals) catalytic nanoparticles. We will obtain more accurate kinetic parameters of reaction intermediates, especially the C2+ oxygenate intermediates using quantum chemical calculations. Exploit catalyst synthesis techniques to better control nanoparticle size, shape, composition, dopant island size, and distribution of steps, edges, corners, defects, and terraces as well as the role of various supports.

Project Details

Start Date
2012-10-01
End Date
2013-09-30
Status
Closed

Team

Principal Investigator

Karl Albrecht
Institution
Archer Daniels Midland Company

Team Members

David Cantu Cantu
Institution
Pacific Northwest National Laboratory

Malsoon Lee
Institution
Pacific Northwest National Laboratory

Libor Kovarik
Institution
Pacific Northwest National Laboratory

Tamas Varga
Institution
Environmental Molecular Sciences Laboratory

Mark Gerber
Institution
Pacific Northwest National Laboratory

Roger Rousseau
Institution
Pacific Northwest National Laboratory

Vassiliki-Alexandra Glezakou
Institution
Pacific Northwest National Laboratory

Mark Engelhard
Institution
Environmental Molecular Sciences Laboratory

Bruce Arey
Institution
Pacific Northwest National Laboratory