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<b style="font-size: 12pt; text-indent: 0in; color: inherit; font-style: inherit; font-variant-ligatures: inherit; font-variant-caps: inherit;"><span style="font-size:14.0pt; color:#0D0D0D">NAME</span></b><b style="font-size: 12pt; text-indent: 0in; color: inherit; font-style: inherit; font-variant-ligatures: inherit; font-variant-caps: inherit;"><span style="font-size:14.0pt; color:#005A58">
</span></b><span style="font-family: "Times New Roman", serif; text-indent: 0in; font-size: 14pt; color: rgb(13, 13, 13);">Rajat Ghosh</span><br>
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<b><span style="font-size:14.0pt; color:black">COMMITTEE CHAIR: </span></b><span style="font-size:14.0pt; color:black">Dr. Michael P Harold</span></p>
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<b><span style="font-size:14.0pt; color:black">DATE: </span></b><span style="font-size:14.0pt; color:black">Monday, December 07, 2020</span></p>
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<b><span style="font-size:14.0pt; color:black">TIME: </span></b><span style="font-size:14.0pt; color:black">10:00 AM (CST)</span></p>
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<b><span style="font-size:14.0pt; color:black">TITLE: </span></b></p>
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<b><span style="font-size:16.0pt; text-transform:uppercase">Enhanced Selective Oxidation of NH<sub>3</sub> in a P</span></b><b><span style="font-size:16.0pt">t<span style="text-transform:uppercase">/A</span>l<sub><span style="text-transform:uppercase">2</span></sub><span style="text-transform:uppercase">O<sub>3</sub>@Cu-ZSM-5
Core-Shell Catalyst and NH<sub>3</sub> Oxidation Rate Kinetic Study over P</span>t<span style="text-transform:uppercase">/A</span>l<sub><span style="text-transform:uppercase">2</span></sub><span style="text-transform:uppercase">O<sub>3</sub></span></span></b></p>
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<b><u><span style="font-size:16.0pt; line-height:200%">Abstract</span></u></b></p>
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The ammonia slip catalyst (ASC) is an essential final step in the emission control system and involves the selective oxidation of NH<sub>3</sub> to N<sub>2</sub>. The state-of-the-art ASC has a dual-layer architecture comprised of a Pt/Al<sub>2</sub>O<sub>3</sub>
(PGM) bottom layer and a metal (Fe, Cu)-exchanged zeolite (M-Z) top layer. The first part of the project deals with the challenges of reducing the PGM loading and ASC volume while enhancing low temperature activity. This is done by scaling down the dual-layer
concept to the level of a single core-shell catalyst particle, Pt/Al<sub>2</sub>O<sub>3</sub>@Cu/ZSM-5, comprised of a PGM core and M-Z shell. The core-shell catalyst had an equivalent activity to that of a conventional Pt/Al<sub>2</sub>O<sub>3</sub> catalyst
containing 3-times higher Pt loading. The core-shell catalyst showed exceptional NH<sub>3</sub> oxidation activity and N<sub>2</sub> selectivity.
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<span style="line-height:150%">The second part of the research is to investigate the NH<sub>3</sub> oxidation kinetics over Pt/Al<sub>2</sub>O<sub>3</sub> catalysts under atmospheric conditions for a wide range of NH<sub>3</sub> concentration. We were able
to show the non-monotonic reaction rate as a function of NH<sub>3</sub> concentration for Pt/Al<sub>2</sub>O<sub>3</sub> catalysts in presence of excess oxygen. We also showed the variation in reaction order from positive to negative order with zero order
reaction at maximum reaction rate. Milling of Pt/Al<sub>2</sub>O<sub>3</sub> resulted in enhanced NH<sub>3</sub> oxidation activity. A microkinetic model with site-competition was developed which could predict the variation in reaction rate and order of the
reaction. </span></p>
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<span style="line-height:150%">The final part of the research deals with the development of a working model for the core-shell catalyst with the microkinetics derived from the kinetic study over Pt/Al<sub>2</sub>O<sub>3</sub> and along with multi-step</span>
SCR <span style="line-height:150%">kinetic formulations to simulate the ASC performance of the Pt/Al<sub>2</sub>O<sub>3</sub>@Cu/ZSM-5 core-shell catalyst. Using the model we showed an optimized core-shell structure by investigating the ASC performance based
on Pt loading and shell thickness. </span>Finally, we discuss the scope of the future work based on our results and observations.</p>
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