Hill, JosephineLiew, Sip Chen2014-09-242014-11-172014-09-242014http://hdl.handle.net/11023/1807One of the ways to dispose of spent carbon-based catalysts is gasification. In this study, the kinetics of CO2 gasification of Ni/activated carbon (AC) catalysts, produced from petroleum coke, were investigated at 700-900 °C using a thermogravimetric analyzer (TGA). The catalysts were coked by exposure to ethylene at 400-600 °C and/or impregnated with ~3.5 and 8.5 wt% vanadium, which is typically deposited during hydrodemetalization (HDM) of heavy oil. The gasification rates of all samples were 30-400 times greater than the rate of gasification of uncatalyzed (i.e., no metal) AC. Rate profiles as a function of conversion were different for all samples, which suggested that nickel was promoted/inhibited as a gasification catalyst in different ways depending on the composition of the sample. Transmission electron microscopy was used to analyze samples before and after gasification. The particle morphologies and chemical analysis (energy dispersive X-ray) help to explain the different gasification behaviours. In particular, the nickel particles on the coked Ni/AC sample became encapsulated by graphite and sintered over time from 20 nm initially to 150 nm after 80% conversion (~10 min at 900 °C). After preparation at 500 °C, the AC support was decorated with ~10 nm nickel particles and wetted with a layer of vanadium. After heating to 900 °C, however, sintering of both metals was evident as well as the formation of new vanadium species including vanadium carbide. The interaction between nickel and vanadium lowered the initial gasification rate but also slowed the deactivation of the nickel.engUniversity of Calgary graduate students retain copyright ownership and moral rights for their thesis. You may use this material in any way that is permitted by the Copyright Act or through licensing that has been assigned to the document. For uses that are not allowable under copyright legislation or licensing, you are required to seek permission.Engineering--ChemicalCO2 gasificationspent catalystsActivated carbonpetroleum cokeNickelvanadiumcoke depositionmaster thesis10.11575/PRISM/26466