Computer Simulation of Chemical Reactions in Porous Materials

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dc.contributor.advisor Gregory N. Parsons, Committee Member en_US
dc.contributor.advisor Keith E. Gubbins, Committee Chair en_US
dc.contributor.advisor Carol K. Hall, Committee Member en_US
dc.contributor.advisor George W. Roberts, Committee Member en_US Turner, Christoffer Heath en_US 2010-04-02T18:35:23Z 2010-04-02T18:35:23Z 2002-08-21 en_US
dc.identifier.other etd-08142002-225425 en_US
dc.description.abstract Understanding reactions in nanoporous materials from a purely experimental perspective is a difficult task. Measuring the chemical composition of a reacting system within a catalytic material is usually only accomplished through indirect methods, and it is usually impossible to distinguish between true chemical equilibrium and metastable states. In addition, measuring molecular orientation or distribution profiles within porous systems is not easily accomplished. However, molecular simulation techniques are well-suited to these challenges. With appropriate simulation techniques and realistic molecular models, it is possible to validate the dominant physical and chemical forces controlling nanoscale reactivity. Novel nanostructured catalysts and supports can be designed, optimized, and tested using high-performance computing and advanced modeling techniques in order to guide the search for next-generation catalysts - setting new targets for the materials synthesis community. We have simulated the conversion of several different equilibrium-limited reactions within microporous carbons and we find that the pore size, pore geometry, and surface chemistry are important factors for determining the reaction yield. The equilibrium-limited reactions that we have modeled include nitric oxide dimerization, ammonia synthesis, and the esterification of acetic acid, all of which show yield enhancements within microporous carbons. In conjunction with a yield enhancement of the esterification reaction, selective adsorption of ethyl acetate within carbon micropores demonstrates an efficient method for product recovery. Additionally, a new method has been developed for simulating reaction kinetics within porous materials and other heterogeneous environments. The validity of this technique is first demonstrated by reproducing the kinetics of hydrogen iodide decomposition in the gas phase, and then predictions are made within slit-shaped carbon pores and carbon nanotubes. The rate constant is found to increase by a factor of 47 in carbon nanotubes, as compared to the same reaction in the bulk gas phase. Overall, the results of these simulation studies demonstrate improvements in chemical reaction yield and chemical kinetics that are possible by understanding the nature of confined reactions, and applying this knowledge to catalyst design. en_US
dc.rights I hereby certify that, if appropriate, I have obtained and attached hereto a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted is the same as that approved by my advisory committee. I hereby grant to NC State University or its agents the non-exclusive license to archive and make accessible, under the conditions specified below, my thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report. en_US
dc.subject molecule en_US
dc.subject confine en_US
dc.subject simulation en_US
dc.subject nanopore en_US
dc.subject carbon en_US
dc.subject reaction en_US
dc.subject Monte Carlo en_US
dc.subject ACT en_US
dc.subject TST en_US
dc.subject rate en_US
dc.subject RxMC en_US
dc.subject catalysis en_US
dc.subject equilibrium en_US
dc.subject selectivity en_US
dc.title Computer Simulation of Chemical Reactions in Porous Materials en_US PhD en_US dissertation en_US Chemical Engineering en_US

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