(611d) Synthesis and Development of Active Nanomaterials for Tri-Reforming

Authors: 
Sasmaz, E., University of California, Irvine
Lauterbach, J., University of South Carolina
The rising concentration of greenhouse gases in the atmosphere requires new technologies to control CO2 emissions. The catalytic tri-reforming process has been proposed to directly utilize CO2 emissions from a flue gas without the need of CO2 pre-separation step while producing syngas with a suitable H2:CO ratio desired for the Fischer-Tropsch process and methanol synthesis. Tri-reforming process requires a novel catalyst with a high surface area, good redox properties and high O2 storage capacity. It should also be thermally stable between 700°C - 900°C and provide resistance to coke formation.

Nickel-based catalysts are typically used in tri-reforming reactions; however stabilizing Ni particles poses a substantial challenge at high reaction temperatures and under reducing reaction conditions. Ni particles covered with metal oxide shells can stabilize Ni, preventing its deactivation at high reaction temperatures. Little is known about how morphology, composition, and dispersion of Ni particles can influence the activity of the catalyst under tri-reforming conditions.

In this work, highly active and stable Ni@CeO2 and Ni@SiO2 core-shell structures are developed by carefully adjusting their structure and composition. The structures are dispersed over Al2O3 and SiO2 supports and their activity for tri-reforming is tested at various temperatures and feed gas compositions. The catalysts are characterized via electron microscopy, x-ray and infrared spectroscopies. Coupling reaction and characterization experiments performed on the well-designed core-shell nanoparticles provide information about the structure-activity relationship.

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