Nickel-based Catalysts for Gasification of Glucose in Supercritical Water

Publication Year:
2010

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Repository URL:
https://ir.lib.uwo.ca/etd/48; https://ir.lib.uwo.ca/cgi/viewcontent.cgi?article=1104&context=etd
Author(s):
Chowdhury, Muhammad Badrul Islam
Tags:
Catalysis; Hydrogen Production; Supercritical Fluid; Nanomaterials; Characterization; Kinetics; Catalysis and Reaction Engineering
artifact description
Gasification of waste biomass to form hydrogen, H2, is a promising new source of green energy; while providing the additional benefit of treating challenging and hazardous waste streams that pollute the environment. Gasification of biomass in supercritical water (SCW) offers an attractive alternative to avoid the energy intensive drying process. In this approach, biomass is hydrolyzed by water into smaller molecules in the presence of a suitable catalyst. This study was aimed at developing an alumina supported nickel based non-noble metal catalyst suitable for biomass gasification in SCW. A lack of detailed characterization on fresh and spent catalysts in SCW has held back progress in this field and is critical due to the highly unusual properties of SCW at high pressure and temperature compared to ambient water. Typically hydrogen rich gaseous product from gasification of biomass in SCW requires temperatures higher than 700 °C, while low temperature processes (300-500 °C) produce methane rich gases. Use of suitable catalysts can lower the activation energy of the reaction, and hydrogen rich gaseous products can be achieved at low temperatures thus lower the operating cost. Use of suitable catalysts also can reduce the formation of chars and tars formed during the gasification process in SCW. Moreover, non-noble catalysts could be beneficial in terms of availability and cost. A kinetic study of SCW gasification is still under development due to the numerous intermediate and final products and complex reaction pathways. In this research, supercritical water gasification (SCWG) and partial oxidation (SCWPO) of a model biomass compound was studied to produce hydrogen rich syngas at lower temperatures (400-500 °C). In this respect non-noble nickel catalysts were synthesized, evaluated and characterized (fresh and spent) to study the catalyst role in SCWG. The catalysts studied were synthesized via incipient wetness impregnation of metal salts on synthesized θ-alumina nanofibers and commercial gamma alumina (converted to theta) pellets (3mm average diameter) as catalyst supports. To synthesize nano structured catalyst supports (alumina nanofibers); a one-pot sol-gel route in scCO2 was adopted without using any hazardous organic solvents, surfactants or other additives for the first time. Aerogel nano catalysts were also directly synthesized via a sol-gel technique using isopropanol as solvent and supercritical carbon dioxide (scCO2) as the drying agent. In this research, it was found that introduction of oxidant after gasification is beneficial in terms of gaseous products and reducing the chemical oxygen demand (COD) in the liquid effluents. Another