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CATALYTIC METHANE IGNITION OVER FREELY-SUSPENDED PALLADIUM
NANOPARTICLES
by
Tsutomu Shimizu
A Dissertation Presented to the
FACULTY OF THE USC GRADUATE SCHOOL
UNIVERSITY OF SOUTHERN CALIFORNIA
In Partial Fulfillment of the
Requirements for the Degree
DOCTOR OF PHILOSOPHY
(MECHANICAL ENGINEERING)
May 2012
Copyright 2012 Tsutomu Shimizu
Object Description
| Title | Catalytic methane ignition over freely-suspended palladium nanoparticles |
| Author | Shimizu, Tsutomu |
| Author email | tsutomus@usc.edu;tsutomu.shimizu@gmail.com |
| Degree | Doctor of Philosophy |
| Document type | Dissertation |
| Degree program | Mechanical Engineering |
| School | Viterbi School of Engineering |
| Date defended/completed | 2012-03-27 |
| Date submitted | 2012-04-26 |
| Date approved | 2012-04-26 |
| Restricted until | 2012-04-26 |
| Date published | 2012-04-26 |
| Advisor (committee chair) | Wang, Hai |
| Advisor (committee member) |
Ronney, Paul D. Campbell, Charles S. Tsotsis, Theodore T. |
| Abstract | Methane ignition catalyzed by palladium (Pd) nanoparticles (NPs) finely dispersed in a CH₄-O₂-N₂ mixture was examined both experimentally and numerically. The ignition experiments were carried out using a temperature-programmed aerosol flow reactor wherein a catalyst precursor was injected into the flow reactor in a form of aerosol generated through a miniature nebulizer. The kinetics of nanoparticle formation was examined using time-resolved microprobe-sampling measurements along with mobility sizing. The morphology and the chemical composition of the NPs were identified by the transmission electron microscopy and the x-ray photoelectron spectroscopy analyses. A microkinetic gas-surface model of methane oxidation over Pd surface was developed ensuring thermodynamic consistency. The proposed model was validated against the aerosol flow reactor experiment as well as the literature stagnation flow reactor experiments for H₂-O₂ mixtures. Adiabatic-isobaric ignition delay time calculations performed using the proposed gas-surface model suggests that fuel ignition occurs through a two-stage process of heat release due to catalysis followed by gas-phase reactions. Guidelines toward optimum atomistic design of nanocatalyst are discussed. |
| Keyword | catalytic combustion; palladium; nanoparticles; surface reactions; flow reactor; ignition delay times; methane ignition |
| Language | English |
| Part of collection | University of Southern California dissertations and theses |
| Publisher (of the original version) | University of Southern California |
| Place of publication (of the original version) | Los Angeles, California |
| Publisher (of the digital version) | University of Southern California. Libraries |
| Provenance | Electronically uploaded by the author |
| Type | texts |
| Legacy record ID | usctheses-m |
| Rights | Shimizu, Tsutomu |
| Access conditions | The author retains rights to his/her dissertation, thesis or other graduate work according to U.S. copyright law. Electronic access is being provided by the USC Libraries in agreement with the author, as the original true and official version of the work, but does not grant the reader permission to use the work if the desired use is covered by copyright. It is the author, as rights holder, who must provide use permission if such use is covered by copyright. The original signature page accompanying the original submission of the work to the USC Libraries is retained by the USC Libraries and a copy of it may be obtained by authorized requesters contacting the repository e-mail address given. |
| Repository name | University of Southern California Digital Library |
| Repository address | USC Digital Library, University of Southern California, University Park Campus MC 7002, 106 University Village, Los Angeles, California 90089-7002, USA |
| Repository email | cisadmin@usc.edu |
| Archival file | uscthesesreloadpub_Volume4/etd-ShimizuTsu-656.pdf |
Description
| Title | Page 1 |
| Full text | CATALYTIC METHANE IGNITION OVER FREELY-SUSPENDED PALLADIUM NANOPARTICLES by Tsutomu Shimizu A Dissertation Presented to the FACULTY OF THE USC GRADUATE SCHOOL UNIVERSITY OF SOUTHERN CALIFORNIA In Partial Fulfillment of the Requirements for the Degree DOCTOR OF PHILOSOPHY (MECHANICAL ENGINEERING) May 2012 Copyright 2012 Tsutomu Shimizu |
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