In-situ MAS NMR Investigations on Catalytic Conversion of Biogenic Molecules in the Presence and Absence of Water
EMSL Project ID
47841
Abstract
The catalyzed conversion of biomass to hydrocarbon energy carriers requires a cascade of reactions that deconstruct and reduce the polymeric, highly oxofunctionalized biomass material. This chemistry faces steep challenges, as it has to be performed in an aqueous environment under conditions that are highly corrosive towards catalysts. The anticipated scale of the transformations demands that the complex catalysts involved be highly efficient, stable, regenerable, and economically viable heterogeneous catalysts. Currently, none of the known catalysts meets these requirements. In order to develop new catalysts satisfying these requirements, a fundamental understanding of the active centers, reaction intermediates and reaction dynamics/kinetics associated with the multi-step conversion of biomass related polar molecules, i.e., the precursor molecules to fuels, on multifunctional catalytic surfaces using a range of model catalysts is critically needed. We propose to use our unique in situ magic angle spinning (MAS) NMR capabilities that have been or are being developed by the primary author and his collaborators, combined with computational modeling of NMR parameters, to carry out fundamental studies to understand the surface chemistry of metal oxide catalysts useful for individual reactions in biomass conversion, and the effects of water on the reactivity and stability of these catalytic materials. Specifically, we will use a range of model catalysts, containing either supported or unsupported metal oxides with varying acid/base and redox chemical properties, including oxides composed of pre-formed molecular cluster ions with well?defined geometrical structures such as the polyoxometallates (POMs) with an initial emphasis on PW12 materials with the Keggin structure. Besides in situ NMR and computational modeling, we will also use EMSL's advanced imaging and other spectroscopy capabilities, such as TEM, SEM and XPS to study the surface morphology of the spent catalysts from the NMR reactor after the in situ NMR analysis.
Project Details
Project type
Large-Scale EMSL Research
Start Date
2013-10-01
End Date
2015-09-30
Status
Closed
Released Data Link
Team
Principal Investigator
Co-Investigator(s)
Team Members
Related Publications
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