Saroj Pradhan

Date of Graduation

2017

Document Type

Dissertation

Degree Type

PhD

College

Statler College of Engineering and Mineral Resources

Department

Mechanical and Aerospace Engineering

Committee Chair

Arvind Thiruvengadam

Committee Co-Chair

Marc C Besch

Committee Member

Mario Perhinschi

Committee Member

Ross Ryskamp

Committee Member

Bharadwaj Shathiamoorthy

Abstract

Three-way catalyst (TWC) equipped stoichiometric natural gas vehicles have proven to be an effective alternative fuel strategy that shows significant low NOx emissions characteristics. However, recent studies have shown the TWC activity to contribute to elevated levels of tailpipe ammonia (NH 3) emissions. Although a non-regulated pollutant, ammonia is a potent pre-cursor to ambient secondary PM formation. Ammonia is an inevitable byproduct of fuel rich operation that results in lowest NOx slip through the TWC after-treatment system.;The main objective of the study is to develop a passive Ammonia Reduction Catalyst (passive-ARC) based NH3 reduction strategy that results in an overall reduction of ammonia as well as NOx emissions. The study investigated the characteristics of Fe-based and Cu-based zeolites SCR catalysts in storage and desorption of ammonia at high exhaust temperature conditions, that are typical of stoichiometric natural gas engines. Continuous measurements of NOx and NH3 before and after the SCR systems were conducted using a Fourier Transform Infrared Spectrometry (FTIR) gas analyzer. Results of the investigation showed that both, the Fe- and Cu zeolite SCRs adsorbed above 90% of TWC generated NH3 emissions below 350--375 °C SCR temperatures. Desorption or slipping of NH3 was observed at exhaust gas temperatures exceeding 400 °C. In terms of NOx conversions, Fe-zeolite showed efficiency between 50--80% above temperatures of 300--350 °C while Cu-zeolite performed well at lower SCR temperature from 250 °C and above with a conversion efficiency of greater than 50%.;In order to efficiently reduce both NOx and NH3 simultaneously over longer durations it was found that an engine-based air fuel ratio operation strategy for the passive-ARC system must be developed. To this extent, the study extended its objectives to develop an engine-based control strategy that results in stoichiometric ammonia production operation followed by brief lean operation to regenerate the saturated ammonia reduction catalyst using high NOx slip through TWC. The study presents comprehensive results of ammonia storage characteristics of SCRs pertaining to stoichiometric natural gas engine exhaust as well as an advanced engine control strategy approach to simultaneously reduce both NOx and NH3 using an alternating air -fuel ratio approach.

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