In-situ Transient Studies on Supported Noble Metal Catalysts PDF Download
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Author: Yao-En Li
Publisher:
ISBN:
Category :
Languages : en
Pages : 288
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Book Description
Author: Yao-En Li
Publisher:
ISBN:
Category :
Languages : en
Pages : 288
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Book Description
Author: Keishla R. Rivera-Dones
Publisher:
ISBN:
Category :
Languages : en
Pages : 0
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Catalytically driven processes account for over ninety percent of industrial chemical manufacturing today. Developments in manufacturing processes are largely driven by continued improvements in catalytic materials, which aim to increase production volumes while minimizing costs along with safety and environmental hazards. In order to achieve these goals, however, a rational approach in catalyst design must be pursued that aims to understand and build upon the fundamental structural, electronic, and chemical properties governing catalytic performance. To that purpose, the work presented in this dissertation makes use of kinetic experiments, theoretical models, and advanced characterization techniques to generate a fundamental understanding of noble metal surfaces employed in a variety of catalytic reaction systems. In Chapter 2, we discuss the use of N2 physisorption, CO chemisorption, and NH3 temperature programed desorption to evaluate the effect of support acidity on the reactivity profiles of various zeolite-supported Pt and Pt-Sn catalysts for the non-oxidative coupling of methane to ethylene and aromatics. Reactivity studies for Pt-Sn/H-ZSM-5 catalysts at 973 K showed that, while all catalysts produced ethylene as the primary product, increasing support acidity led to an increase in naphthalene selectivity at the expense of benzene selectivity. Volcano-shaped profiles observed for the generation of aromatic products suggest that the formation of a reactive hydrocarbon pool on acidic support surfaces could be responsible for the oligomerization of ethylene. Notably, the Pt-Sn/H-ZSM-5 (SiO2:Al2O3 = 50) catalyst was found to be comparable to the state-of-the-art Mo/H-ZSM-5 catalysts in terms of carbon product generation and resistance to coke formation. In Chapter 3, x-ray absorption spectroscopy (XAS) was used to highlight the effect of local electronic and structural environments in specially synthesized metallic catalysts. The local coordination and nearest-neighbor distance of Pd species were evaluated to understand metal dispersion and the effect of catalyst support on the extent of bimetallic particle formation in Pd, AgPd, CuPd, and AuPd catalysts synthesized by controlled surface reactions (CSR) for a variety of amination, hydrodechlorination, and hydrogenation reactions. Near-edge structure analyses were also used on these Pd catalysts, as well as on a set of Mo-containing multi-metallic catalysts prepared by atomic layer deposition (ALD) for synthesis gas conversion, to understand catalyst reducibility along with potential support and hydrogen spillover effects on the extent of metal reduction. Chapter 4 evaluates the effects of catalyst support and pretreatment conditions on the hydrogenation of acetone over SiO2-, Al2O3-, and ZSM-5-supported platinum catalysts. Pt/ZSM-5 catalysts were found to have specific conversion rates and turnover frequencies that were 2 - 3 orders of magnitude higher than those observed over Pt/SiO2 and Pt/Al2O3 catalysts, regardless of zeolite acidity or pretreatment conditions. For Pt/ZSM-5 catalysts, the higher activity was achieved by increasing calcination and decreasing reduction temperatures, likely due to the effects of these treatments on the morphology of the platinum particles. CO-FTIR measurements showed a shift to higher frequencies of the Pt-CO band in Pt/ZSM-5 catalysts compared to Pt/SiO2, which alluded to the interactions between Pt and the porous zeolite structure as a source of the activity enhancements observed. Chapter 5 introduces the use of transient kinetics studies and theoretical modeling to explore the importance of surface coverage effects in the hydrogenation of acetone over platinum. Transient models based on steady-state microkinetics using static and dynamic inclusion of surface coverage via the Langmuir and Bragg-Williams approximations, respectively, predicted notable differences in the decay profiles of the most abundant reactive intermediate (MARI) from the catalytic surface. Experimental studies using steady-state isotopic transient kinetic analysis (SSITKA) methods served to validate the theoretical predictions for transients induced by complete acetone removal from or its substitution in the reactant feed and provided tangible evidence for the importance of surface coverage effects in understanding the reactivity of platinum catalysts for acetone hydrogenation. Lastly, Chapter 6 addresses possible future research directions in the field of transient kinetics studies.
Author: Peter Gray
Publisher: Manchester University Press
ISBN: 9780719024511
Category : Chemical equilibrium
Languages : en
Pages : 802
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Book Description
The results of an International Conference on [title] held in Brussels, Belgium, Aug./Sept. 1987, these papers deal with self-organization and nonlinear dynamics in chemistry, giving the results of recent experiments and bringing new emphasis on spatial inhomogeneities and dynamical phenomena in con"
Author: Felix Hemmingsson
Publisher:
ISBN: 9789179054601
Category : Hydrogenation
Languages : en
Pages :
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Author:
Publisher:
ISBN:
Category : Dissertations, Academic
Languages : en
Pages : 810
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Author: Michel Che
Publisher: John Wiley & Sons
ISBN: 3527645330
Category : Technology & Engineering
Languages : en
Pages : 1313
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Book Description
This two-volume book provides an overview of physical techniques used to characterize the structure of solid materials, on the one hand, and to investigate the reactivity of their surface, on the other. Therefore this book is a must-have for anyone working in fields related to surface reactivity. Among the latter, and because of its most important industrial impact, catalysis has been used as the directing thread of the book. After the preface and a general introduction to physical techniques by M. Che and J.C. Vedrine, two overviews on physical techniques are presented by G. Ertl and Sir J.M. Thomas for investigating model catalysts and porous catalysts, respectively. The book is organized into four parts: Molecular/Local Spectroscopies, Macroscopic Techniques, Characterization of the Fluid Phase (Gas and/ or Liquid), and Advanced Characterization. Each chapter focuses upon the following important themes: overview of the technique, most important parameters to interpret the experimental data, practical details, applications of the technique, particularly during chemical processes, with its advantages and disadvantages, conclusions.
![In Situ Infared [i.e. Infrared] Studies of Catalytic Partial Oxidation PDF](https://books.google.com/books/content/images/frontcover/IC58AQAACAAJ?fife=w80-h100)
Author: Chundi Cao
Publisher:
ISBN:
Category :
Languages : en
Pages :
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Catalytic partial oxidation (CPO) has received considerable interest recently both as a way to utilize remote natural gas resources and to provide H[subscript]2 for a fuel cell. Studies on the reactions at lower temperatures and transient conditions were performed, which can provide insights on the mechanism of CPO at high reactions, particularly on the role of the chemical and physical state of the noble metal catalyst. In this work, ignition of methane CPO on Pt/Al[subscript]2O[subscript]3 and Rh/Al[subscript]2O[subscript]3 catalysts and methanol CPO on Pt/Al[subscript]2O[subscript]3 catalysts were studied using in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS). The ignition mechanism study of CH4 on Pt/Al[subscript]2O[subscript]3 showed that oxygen mainly covers the surface until ignition. Competition between the two reactants is assumed. The heat of adsorption of oxygen is a key factor for ignition of the methane partial oxidation reaction on Pt/Al[subscript]2O[subscript]3. The ignition mechanism on Rh/Al[subscript]2O[subscript]3 was found to be different from Pt/Al[subscript]2O[subscript]3. The oxidation state of the catalyst changed significantly as the temperature was raised towards the ignition. An oxidized rhodium state, Rh[superscript]n+, progressively formed as the temperature was increased while Rh[superscript]0 decreased. In addition, a greater amount of Rh[supercript]n+ was found when the oxygen concentration in the feed was higher. From these results, it is hypothesized that ignition of methane CPO on Rh/Al[subscript]2O[subscript]3 is related to the accumulation of the Rh[superscript]n+ state. Dissociation adsorption of methanol occurs on both Al2O3 and Pt/Al[subscript]2O[subscript]3. It is suggested that formate was one of the important intermediates in the reaction pathway. Oxygen species play a key role in the formation of formate on the catalysts, and it also affects the product composition. Formate mainly decomposed into CO, which is the dominant source for CO[subscript]2 production in the reactions at higher temperatures.
Author: Franklin Tao
Publisher: Royal Society of Chemistry
ISBN: 1782621032
Category : Technology & Engineering
Languages : en
Pages : 285
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Book Description
Catalysis is a central topic in chemical transformation and energy conversion. Thanks to the spectacular achievements of colloidal chemistry and the synthesis of nanomaterials over the last two decades, there have also been significant advances in nanoparticle catalysis. Catalysis on different metal nanostructures with well-defined structures and composition has been extensively studied. Metal nanocrystals synthesized with colloidal chemistry exhibit different catalytic performances in contrast to metal nanoparticles prepared with impregnation or deposition precipitation. Additionally, theoretical approaches in predicting catalysis performance and understanding catalytic mechanism on these metal nanocatalysts have made significant progress. Metal Nanoparticles for Catalysis is a comprehensive text on catalysis on Nanoparticles, looking at both their synthesis and applications. Chapter topics include nanoreactor catalysis; Pd nanoparticles in C-C coupling reactions; metal salt-based gold nanocatalysts; theoretical insights into metal nanocatalysts; and nanoparticle mediated clock reaction. This book bridges the gap between nanomaterials synthesis and characterization, and catalysis. As such, this text will be a valuable resource for postgraduate students and researchers in these exciting fields.
Author: Dilip Kumar Paul
Publisher:
ISBN:
Category : Chemical reactions
Languages : en
Pages : 428
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Book Description
Author: Alexis T. Bell
Publisher:
ISBN:
Category : Science
Languages : en
Pages : 364
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Book Description
Good,No Highlights,No Markup,all pages are intact, Slight Shelfwear,may have the corners slightly dented, may have slight color changes/slightly damaged spine.
