Date of Award

January 2016

Degree Type

Dissertation

Degree Name

Doctor of Philosophy (PhD)

Department

Chemical Engineering

First Advisor

Fabio H. Ribeiro

Second Advisor

W. Nicholas Delgass

Committee Member 1

Jeffrey P. Greeley

Committee Member 2

Jeffrey T. Miller

Committee Member 3

Aleksey Yezerets

Abstract

Increasingly stringent regulations to reduce emissions of nitrogen oxides (NOx) from exhausts of heavy-duty diesel engines has set the stage to delve into a detailed investigation of engine after-treatment catalysts in order to understand the chemistry during their operation and design the next generation of catalytic formulations to meet future requirements. Small-pore Cu- and Fe-exchanged SSZ-13 catalysts with chabazite (CHA) topology are able to sustain high catalytic rates for selective catalytic reduction (SCR) even after exposure to harsh hydrothermal conditions present in diesel exhaust. Probing the redox behavior and the active site requirements for standard SCR on Cu-SSZ-13 catalysts using a combination of infrared (FTIR) and x-ray absorption (XAS) spectroscopies, kinetic measurements and density functional theory (DFT) calculations forms the basis for this dissertation.

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