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<b><span style="font-size:14.0pt; font-family:"Times New Roman",serif">NAME: </span>
</b><span style="font-size:14.0pt; font-family:"Times New Roman",serif">Hari Narayanan Thirumalai</span><span style="font-family:"Times New Roman",serif"></span></p>
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<span style="font-size:14.0pt; font-family:"Times New Roman",serif"> </span><span style="font-family:"Times New Roman",serif"></span></p>
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<b><span style="font-size:14.0pt; font-family:"Times New Roman",serif">DATE: </span>
</b><span style="font-size:14.0pt; font-family:"Times New Roman",serif">Tuesday, November 19, 2019</span><span style="font-family:"Times New Roman",serif"></span></p>
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<b><span style="font-size:14.0pt; font-family:"Times New Roman",serif">TIME: </span>
</b><span style="font-size:14.0pt; font-family:"Times New Roman",serif">9:00 A.M.</span><span style="font-family:"Times New Roman",serif"></span></p>
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<b><span style="font-size:14.0pt; font-family:"Times New Roman",serif">PLACE:</span></b><span style="font-size:14.0pt; font-family:"Times New Roman",serif"> Chemical Engineering Conference Room</span><span style="font-family:"Times New Roman",serif"></span></p>
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<b><span style="font-size:14.0pt; font-family:"Times New Roman",serif">CHAIR/ADVISOR:
</span></b><span style="font-size:14.0pt; font-family:"Times New Roman",serif">Dr. Lars Grabow</span><span style="font-family:"Times New Roman",serif"></span></p>
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<b><span style="font-size:14.0pt; line-height:105%; font-family:"Times New Roman",serif">TITLE:</span></b><span style="font-family:"Times New Roman",serif"></span></p>
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<b><span style="font-size:14.0pt; line-height:105%; font-family:"Times New Roman",serif">Integrated Theoretical and Transient Kinetic Investigation of Catalytic Materials for the Selective Synthesis of Hydrogen and Aromatic Hydrocarbons</span></b></p>
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<span style="font-family:"Times New Roman",serif">Metal-exchanged zeolites are emerging as catalytic materials containing isolated metal centers that perform chemical transformation with high activity and selectivity to desired products. While there exist very
successfully commercialized examples, for instance Cu-SSZ-13 for automotive emissions applications, much is unknown about metal sites in zeolites. Thus, statistical analyses of energetic quantities obtained from density functional theory (DFT) simulations
of various zeolite models were performed for the activation of methane as probe hydrocarbon species. A comprehensive error analysis overwhelmingly shows that the identity and type of metal species in the zeolite determines the reactivity rather than the zeolite
framework properties. Statistical distributions were used to identify and validate other metals that would theoretically function as catalysts for methane activation.</span></p>
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<span style="font-family:"Times New Roman",serif">Insights gained from the investigation of a diverse set of metal-exchanged zeolites were applied in understanding the mechanisms by which Ag-ZSM-5 enhances the selective formation of aromatic hydrocarbons from
ethylene. Silver sites in the zeolite were experimentally and computationally characterized as Ag cations. Transient pulsing experiments using the temporal analysis of products (TAP) reactor and exploration of reaction mechanisms using DFT reveal that silver
sites catalyze dehydrogenation and hydrogen-transfer pathways and accelerate the accumulation of aromatic hydrocarbon forming precursors. The cause for the enhancement of these chemistries arises from the synergistic Brønsted–Lewis acid character of the zeolite.</span></p>
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<span style="font-family:"Times New Roman",serif">The TAP technique was used to understand the finer aspects of the methylation of toluene to xylene, both important aromatic hydrocarbons. Pulse responses of reactants and products provide insights on competitive
adsorption inside the zeolite, with methanol and methanol-based intermediates of finite lifetime identified as being crucial to the process of methylation. Typically in industry, hydrocarbon conversion processes using zeolites include co-feeds of hydrogen
that are usually obtained from methane steam-reforming, a highly capital and energy intensive process. The search for hydrogen production avenues that do not rely on fossil resources has led to a surge of research devoted to electrocatalytic processes. This
dissertation also explores the surface science of electrocatalytic hydrogen production over novel metal-phosphide surfaces. Density functional theory calculations reveal that metal-rich surface sites catalyze hydrogen evolution, as opposed to accepted notions
that phosphorous-rich sites are the active sites.</span></p>
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