Dissociation of manganese(III) oxide as part of a thermochemical water splitting cycle | | Posted on:2009-12-15 | Degree:Ph.D | Type:Dissertation | | University:University of Colorado at Boulder | Candidate:Francis, Todd Michael | Full Text:PDF | | GTID:1441390002991621 | Subject:Engineering | | Abstract/Summary: | PDF Full Text Request | | A three-step thermochemical cycle to produce renewable hydrogen was proposed, which utilizes manganese(III) oxide and thermal energy to produce hydrogen. Most work on the cycle has focused on the hydrogen generating and product recovery steps with little work on the dissociation. It is essential to understand the dissociation because the feasibility of the cycle is based on this reaction having a high conversion. Because of the importance of the reduction step, this reaction has been selected as the topic of this dissertation. Additionally, because the dispersion of Mn2O3 particles into an Aerosol Flow Reactor (AFR) is important, feeding concepts were developed as well.;Two powder feeding systems were developed: a Spinning Wheel Feeder (SWF) and a Fluidized Bed Feeder (FBF). Results of statistical particle size distribution studies indicated that the FBF was the better choice to disperse Mn2O3 powder. Additionally, results in an AFR demonstrated that the FBF was able to produce higher dissociation conversions.;A study in a Thermogravimetric Analyzer (TGA) indicated multiple mechanisms were controlling Mn2O3 dissociation. The first half reaction of the dissociation was calculated to be controlled by an Avrami-Erofeev mechanism and had an activation energy of 106.4+/-1.9 kJ/mol. The second half reaction had a duel mechanism utilizing an Avrami-Erofeev and Order of Reaction (OOR) mechanism. The mechanisms had activation energies of 251.2+/-6.5 and 110.7+/-24.6 kJ/mol respectively.;Mn2O3 dissociation investigations were done in an AFR. They revealed oxygen is a significant factor and to effectively control the dissociation with temperature and gas flow rate, the oxygen concentration must be below 0.25%. Experimental runs that had oxygen concentrations less than 0.25% were used to calculate reaction rate constants. The Avrami-Erofeev mechanisms were combined into a single mechanism. Rate constants for the Avrami-Erofeev and OOR mechanisms were 1.8E7+/-1.3E7 and 5.6E3+/-4.1E3 s -1 respectively.;The results of a CFD model compared favorably with what was observed experimentally. A heavy feed concentration case predicted this as well. When the gas flow rate was higher the r-velocity was concluded to transport the more reacted powder near the wall to the center of the reactor, leading to higher conversions for the high gas flow rate. | | Keywords/Search Tags: | Dissociation, Gas flow rate, Cycle | PDF Full Text Request | Related items |
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