(557b) Development of Nanoparticle Catalyst for the Trireforming of CO2-Rich Flue Gases

Today’s chemical industry is very complex with most commodity chemicals being produced from some variation of petroleum feedstocks.  From transportation fuels to polymers, petroleum is truly the largest source of basic hydrocarbons for which many of the common household products consumers use.  Along with this, stems many industrial and environmental issues which must be addressed for long-term stability of the industry.  Upgrading of these crude feedstocks requires hydrogen, generally supplied via steam methane reforming (SMR).  Hydrogen is typically produced via methane steam reforming reactions.  Carbon dioxide, noted for its greenhouse gas potential, is produced as a byproduct of methane steam reforming.  CO₂ sequestration is a growing concern and is at the forefront of many political and environmental policies that are being introduced worldwide.  One avenue to combat the growing release of CO₂ into the atmosphere is to convert it to useful chemicals via trireforming.

            Trireforming is the conversion of carbon dioxide, methane, and water to produce synthesis gas (syngas).  The uniqueness of the trireforming technology is that bulk flue gases can be utilized without the separation of CO₂ and steam.  The problems associated with the conversion of CO₂ are overcoming thermodynamic limitations, as carbon dioxide tends to be a very stable molecule.  However, through careful catalyst design, a novel catalyst has been synthesized that utilizes reverse micelle technology to create highly active nano-sized nickel particles onto metal-oxide supports.  In terms of catalyst reactivity, selectivity, and robustness, a mixed metal oxide consisting of Magnesia and titania oxides is the best performing support.  Reverse micelles using sodium dioctyl succinate surfactant allow for metal deposition down to 20 nm sized nickel particles.             

            Our laboratory has developed some novel trireforming catalysts that are capable of extending our carbon resources with high conversion performance.  Characterizations of the catalyst have been performed using Scanning Electron Microscopy, X-ray Diffraction, Temperature Programmed Reaction (and Desorption), and in situ FTIR microscopy. Trireforming reaction temperatures of 800°C have been reported in the literature.  According to the results supported by our catalyst characterization efforts, reaction temperatures of 700°C will be sufficient for the H2:CO ratio of 2 required for additional hydrocarbon or methanol synthesis reactions.  These findings and a postulated reaction site mechanism will be presented.