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Atomic-Resolution in situ and operando Visualization of Oxygen Transfer Reactions over CeO2-Supported Pt Catalysts.

紀錄類型:	書目-電子資源 : Monograph/item
正題名/作者:	Atomic-Resolution in situ and operando Visualization of Oxygen Transfer Reactions over CeO2-Supported Pt Catalysts./
作者:	Vincent, Joshua Lawrence.
出版者:	Ann Arbor : ProQuest Dissertations & Theses, : 2021,
面頁冊數:	322 p.
附註:	Source: Dissertations Abstracts International, Volume: 83-03, Section: B.
Contained By:	Dissertations Abstracts International83-03B.
標題:	Chemical engineering. -
電子資源:	http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=28644484
ISBN:	9798535541884

Atomic-Resolution in situ and operando Visualization of Oxygen Transfer Reactions over CeO2-Supported Pt Catalysts.
Vincent, Joshua Lawrence.

Atomic-Resolution in situ and operando Visualization of Oxygen Transfer Reactions over CeO2-Supported Pt Catalysts. - Ann Arbor : ProQuest Dissertations & Theses, 2021 - 322 p.

Source: Dissertations Abstracts International, Volume: 83-03, Section: B.

Thesis (Ph.D.)--Arizona State University, 2021.

This item must not be sold to any third party vendors.

Oxygen transfer reactions are central to many catalytic processes, including those underlying automotive exhaust emissions control and clean energy conversion. The catalysts used in these applications typically consist of metal nanoparticles dispersed on reducible oxides (e.g., Pt/CeO2), since reducible oxides can transfer their lattice oxygen to reactive adsorbates at the metal-support interface. There are many outstanding questions regarding the atomic and nanoscale spatial variation of the Pt/CeO2 interface, Pt metal particle, and adjacent CeO2 oxide surface during catalysis. To this end, a range of techniques centered around aberration-corrected environmental transmission electron microscopy (ETEM) were developed and employed to visualize and characterize the atomic-scale structural behavior of CeO2-supported Pt catalysts under reaction conditions (in situ) and/or during catalysis (operando).A model of the operando ETEM reactor was developed to simulate the gas and temperature profiles during conditions of catalysis. Most importantly, the model provides a tool for relating the reactant conversion measured with spectroscopy to the reaction rate of the catalyst that is imaged on the TEM grid. As a result, this work has produced a truly operando TEM methodology, since the structure observed during an experiment can be directly linked to quantitative chemical kinetics of the same catalyst.This operando ETEM approach was leveraged to investigate structure-activity relationships for CO oxidation over Pt/CeO2 catalysts. Correlating atomic-level imaging with catalytic turnover frequency reveals a direct relationship between activity and dynamic structural behavior that (a) destabilizes the supported Pt particle, (b) marks an enhanced rate of oxygen vacancy creation and annihilation, and (c) leads to increased strain and reduction in the surface of the CeO2 support.To further investigate the structural meta-stability (i.e., fluxionality) of 1-2 nm CeO2-supported Pt nanoparticles, time-resolved in situ AC-ETEM was employed to visualize the catalyst's dynamical behavior with high spatiotemporal resolution. Observations are made under conditions relevant to the CO oxidation and water-gas shift (WGS) reactions. Finally, deep learning-based convolutional neural networks were leveraged to develop novel denoising techniques for ultra-low signal-to-noise images of catalytic nanoparticles.

ISBN: 9798535541884Subjects--Topical Terms:

560457
Chemical engineering.
Subjects--Index Terms:

Catalysts

Atomic-Resolution in situ and operando Visualization of Oxygen Transfer Reactions over CeO2-Supported Pt Catalysts.
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245 1 0 $a Atomic-Resolution in situ and operando Visualization of Oxygen Transfer Reactions over CeO2-Supported Pt Catalysts.
260 1 $a Ann Arbor : $b ProQuest Dissertations & Theses, $c 2021
300 $a 322 p.
500 $a Source: Dissertations Abstracts International, Volume: 83-03, Section: B.
500 $a Advisor: Crozier, Peter A.
502 $a Thesis (Ph.D.)--Arizona State University, 2021.
506 $a This item must not be sold to any third party vendors.
520 $a Oxygen transfer reactions are central to many catalytic processes, including those underlying automotive exhaust emissions control and clean energy conversion. The catalysts used in these applications typically consist of metal nanoparticles dispersed on reducible oxides (e.g., Pt/CeO2), since reducible oxides can transfer their lattice oxygen to reactive adsorbates at the metal-support interface. There are many outstanding questions regarding the atomic and nanoscale spatial variation of the Pt/CeO2 interface, Pt metal particle, and adjacent CeO2 oxide surface during catalysis. To this end, a range of techniques centered around aberration-corrected environmental transmission electron microscopy (ETEM) were developed and employed to visualize and characterize the atomic-scale structural behavior of CeO2-supported Pt catalysts under reaction conditions (in situ) and/or during catalysis (operando).A model of the operando ETEM reactor was developed to simulate the gas and temperature profiles during conditions of catalysis. Most importantly, the model provides a tool for relating the reactant conversion measured with spectroscopy to the reaction rate of the catalyst that is imaged on the TEM grid. As a result, this work has produced a truly operando TEM methodology, since the structure observed during an experiment can be directly linked to quantitative chemical kinetics of the same catalyst.This operando ETEM approach was leveraged to investigate structure-activity relationships for CO oxidation over Pt/CeO2 catalysts. Correlating atomic-level imaging with catalytic turnover frequency reveals a direct relationship between activity and dynamic structural behavior that (a) destabilizes the supported Pt particle, (b) marks an enhanced rate of oxygen vacancy creation and annihilation, and (c) leads to increased strain and reduction in the surface of the CeO2 support.To further investigate the structural meta-stability (i.e., fluxionality) of 1-2 nm CeO2-supported Pt nanoparticles, time-resolved in situ AC-ETEM was employed to visualize the catalyst's dynamical behavior with high spatiotemporal resolution. Observations are made under conditions relevant to the CO oxidation and water-gas shift (WGS) reactions. Finally, deep learning-based convolutional neural networks were leveraged to develop novel denoising techniques for ultra-low signal-to-noise images of catalytic nanoparticles.
590 $a School code: 0010.
650 4 $a Chemical engineering. $3 560457
650 4 $a Nanoscience. $3 587832
650 4 $a Materials science. $3 543314
650 4 $a Research. $3 531893
650 4 $a Principles. $3 3559989
650 4 $a Datasets. $3 3541416
650 4 $a Nanoparticles. $3 605747
650 4 $a Clean technology. $3 3564885
650 4 $a Chemical reactions. $3 519248
650 4 $a Adsorption. $3 580046
650 4 $a Carbon monoxide. $3 738287
650 4 $a Environmental restoration. $3 3564335
650 4 $a Energy. $3 876794
650 4 $a Visualization. $3 586179
650 4 $a Gases. $3 559387
650 4 $a Spectrum analysis. $3 520440
650 4 $a Oxidation. $3 714629
650 4 $a Experiments. $3 525909
650 4 $a Sensors. $3 3549539
650 4 $a Neural networks. $3 677449
650 4 $a Microscopy. $3 540544
650 4 $a Benchmarks. $3 3548256
650 4 $a Kinetics. $3 717752
650 4 $a Catalytic converters. $3 3687977
650 4 $a Catalysis. $3 560465
650 4 $a Geometry. $3 517251
650 4 $a Mars. $3 3687764
653 $a Catalysts
653 $a Ceria
653 $a In situ TEM
653 $a Operando TEM
653 $a Platinum nanoparticles
653 $a Pt/CeO2
690 $a 0794
690 $a 0542
690 $a 0565
690 $a 0791
710 2 $a Arizona State University. $b Chemical Engineering. $3 1682515
773 0 $t Dissertations Abstracts International $g 83-03B.
790 $a 0010
791 $a Ph.D.
792 $a 2021
793 $a English
856 4 0 $u http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=28644484