DOCSLIB.ORG

Frontiers at the Interface of Homogeneous and Heterogeneous Catalysis

Total Page：16

File Type：pdf, Size：1020Kb

Download full-text PDF Read full-text

Load more

FRONTIERS AT THE INTERFACE OF HOMOGENEOUS AND HETEROGENEOUS CATALYSIS Meeting of the Catalysis Science Program Chemical Sciences, Geosciences and Biosciences Division Office of Basic Energy Sciences U.S. Department of Energy Westin Annapolis Annapolis, Maryland June 30 – July 2, 2013 This document was produced under contract number DE-AC05-060R23100 between the U.S. Department of Energy and Oak Ridge Associated Universities. FOREWORD The 2013 Catalysis Science Program Meeting is sponsored by the Division of Chemical Sciences, Geosciences and Biosciences, Office of Basic Energy Sciences (BES), U.S. Department of Energy. It is being held on June 30 through July 2, 2013, at the Westin Annapolis Hotel, Annapolis, Maryland. The purposes of this meeting are to discuss the recent advances in the chemical, physical, and biological bases of catalysis science, to foster exchange of ideas and cooperation among participants, and to discuss the new challenges and opportunities recently emerging in energy technologies. Catalysis activities within BES emphasize fundamental research aimed at initially understanding and finally controlling the chemical conversion of natural and artificial feedstocks. The long-term goal of this research is to discover fundamental principles and produce ever more insightful approaches to predict structure-reactivity behavior. Such knowledge, integrated with advances in chemical and materials synthesis, in situ and operando analytical instrumentation, and chemical kinetics and quantum chemistry methods, will allow the control of chemical reactions along desired pathways. Ultimately, this new knowledge should impact the efficiency of conversion of natural resources into fuels, chemicals, materials, or other forms of energy, while minimizing the impact to the environment. This year’s meeting is focused on three topical areas: (i) the interface of homogeneous and heterogeneous catalysis, (ii) catalysis for biomass or solar energy conversion, and (iii) molecular catalysis, with an emphasis on organic synthesis. Special thanks go to our invited speakers and guest junior scientists, who will expose us to recent advances in their fields; to the program investigators and their students, postdocs, and collaborators, for their dedication to the continuous success and visibility of the BES Catalysis Science Program; and to the session moderators, for their invaluable help. We also thank the Oak Ridge Institute for Science and Education staff for the logistical and web support and the compilation of this volume. Christopher Jones1 and Raul Miranda2 1Georgia Institute of Technology 2Office of Basic Energy Sciences - U.S. Department of Energy i This page is intentionally blank. ii AGENDA Sunday Afternoon and Evening, June 30, 2013 10:00 - on Registration 12:00 - 1:00 pm Lunch and Welcoming Remarks Session I, Moderator: Alex Katz (UC Berkeley) 1:00 – 1:40 pm Invited Speaker: Cristophe Copéret (ETH Zürich) “Controlled Functionalization and Molecular Understanding of Surfaces: Towards Supported Single-Site Catalysts and Beyond” 1:40 – 2:10 pm T. Don Tilley (UC Berkeley, LBNL) “Molecular Routes to Single-Site Catalytic Surface Species for Selective Oxidations” 2:10 – 2:40 pm Steven Tait (Indiana Univ.) “Metal/Organic Surface Catalyst for Low-Temperature Methane Oxidation: Bi-Functional Union of Metal-Organic Complex and Chemically Complementary Surface” 2:40 – 3:10 pm Tobin Marks (Northwestern Univ.) “Supported Organometallic Complexes: Surface Chemistry, Spectroscopy, Catalysis and Homogeneous Models” Session II, Moderator: Ted Betley (Harvard University) 3:30 – 4:00 pm Susannah Scott (UC Santa Barbara) “Exploring the Relationship between Homogeneous and Heterogeneous Reaction Kinetics” 4:00 – 4:30 pm Justin Notestein (Northwestern University) “Templating Routes to Supported Oxide Catalysts by Design” 4:30 – 5:00 pm Liviu Mirica (Washington University –St. Louis) “Novel Palladium Catalysts for the Oxidative Oligomerization of Methane & Carbon Dioxide Reduction” 5:00 – 5:30 pm Aaron Appel (PNNL) “An Energy-Based Approach to Bifunctional Molecular Catalysis for CO2 Reduction and Fuel Utilization” 5:30 - 6:30 pm Dinner Session III, Moderator: Brent Gunnoe (University of Virginia) 6:30 – 7:10 pm Invited Speaker: Huw Davies (Emory University) “Center Approach to C-H Functionalization” iii 7:10 – 7:40 pm Dean Toste (UC Berkeley, LBNL) “Selective Reactions of Carbon-Carbon π-Bonds Catalyzed by Cations and Anions” 7:40 – 8:20 pm Invited Speaker: Scott Miller (Yale University) “Asymmetric Catalysis in Complex Molecular Environments” 8:20 – 10:00 pm Poster Session I (Odd Numbers) Monday Morning, July 1 7:00 - 8:15 am Breakfast Session IV, Moderator: Morris Bullock (PNNL) 8:30 - 9:10 am Invited Speaker: Wenbin Lin (Univ. of Chicago) “Metal- Organic Frameworks as Single Site Solid Catalysts” 9:10 - 9:40 am Larry Que (Univ. of Minnesota) “Bio-inspired Nonheme Iron Catalysts for Hydrocarbon Oxidations” 9:40 - 10:10 am John Hartwig (UC Berkeley–LBNL) “Studies on Homogeneous Catalysis for Efficient Synthesis from Chemical Feedstocks” Session V, Moderator: Mahdi Abu-Omar (Purdue University) 10:30 - 11:10 am Invited Speaker: Noritaka Mizuno (Univ. of Tokyo) “Design of Polyoxometalate-Based Molecular Catalysts for Bridging the Gap between Homogeneous and Heterogeneous Catalysis” 11:10 - 11:40 am Harold Kung (Northwestern University) “Nanoconfinement Effects in Heterogeneous Catalysis” 11:40 - 12:10 pm Geoffrey Coates (Cornell University) “Development and Application of New Carbonylation Catalysts: Improvements in Regioselectivity, Stereoselectivity, Activity and Exploration of New Reactions” 12:10 - 12:40 pm Robert Crabtree (Yale University) “Moving to Nonprecious Metal Catalysis” 12:40 – 2:30 pm Lunch - Networking Monday Afternoon, July 1 Session VI, Moderator: Richard Finke (Colorado State University) 2:30 - 3:10 pm Invited Speaker: Alan Goldman (Rutgers Univ.) “Addition of O-H Bonds to Olefins Catalyzed by Pincer-Iridium Complexes” iv 3:10 – 3:40 pm Malcolm Chisholm (Ohio State Univ.) “Developing s-Block Element Catalysis and New Chemical Transformations” 3:40 - 4:10 pm Christopher Marshall (ANL) “Fundamental Understanding and Control of Selectivity and Deactivation in Biomass Conversion Catalysts” 4:10 – 4:40 pm Eugene Chen (Colorado State Univ.) “Catalytic Conversion of Glucose and Cellulose into HMF and Subsequent Upgrading to Value-Added Chemicals and Liquid Fuels” 4:40 – 5:10 pm Raul Lobo (Univ. of Delaware) “Selective Catalytic Dehydration and Hydrodeoxygenation Reactions for the Production of Fuels and Chemicals from Biomass” 5:10 - 6:20 pm Dinner Monday Evening, July 1 Session VII, Moderator: Bruce Gates (UC Davis) 6:20 - 7:00 pm Johannes Lercher (PNNL, T.U. Munich) “Understanding Elementary Steps of Catalytic Conversions in Water to Achieve Complex Transformations” 7:00 - 7:30 pm Suljo Linic (Univ. of Michigan) “Photo-catalysis on Plasmonic Metal Nanoparticles” 7:30 - 8:00 pm Andreas Heyden (Univ. of South Carolina) “Theoretical Investigation of Heterogeneous Catalysis at the Solid-Liquid Interface for the Conversion of Lignocellulosic Biomass Model Molecules” 8:20 - 10:00 pm Poster Session II (Even Numbers) Tuesday Morning, July 2 7:00 - 8:15 am Breakfast Session VIII, Moderator: Robert Waymouth (Stanford University) 8:30 - 9:00 am Jens Nørskov (SLAC, Stanford Univ.) “Theoretical Description of CO2 Reduction” 9:00 - 9:30 am Aditya Bhan (Univ. of Minnesota) “One-Pot Catalytic Conversion of Biomass and Alkanes: Kinetically Coupling Deoxygenation and Dehydrogenation Pathways” 9:30 - 10:00 am Jose Rodriguez (BNL) “Catalysis: Reactivity and Structure” 10:00 - 10:20 am Coffee Break v Session IX, Moderator: Christopher Jones (Georgia Institute of Technology) 10:50 – 11:20 am Zili Wu (ORNL) “Revealing the Surface Structure of Ceria Nanocrystals with Well-Defined Facets” 11:20 – 11:50 am Will Medlin (Univ. of Colorado) “Selectivity Control through Modification of Metal Catalysts with Organic Monolayers” 11:50 - 2:00 pm Lunch and Discussion – Future Directions vi Table of Contents Foreword ..................................................................................................... i Agenda ....................................................................................................... iii Sunday Afternoon, Session I Invited Speaker: Cristophe Copéret – Controlled Functionalization and Molecular Understanding of Surfaces: Towards Supported Single-Site Catalysts and Beyond .................................................................................... 3 T. Don Tilley – Molecular Routes to Single-Site Catalytic Surface Species for Selective Oxidations ...................................................................................... 4 Steven Tait – Metal/Organic Surface Catalyst for Low-Temperature Methane Oxidation: Bi-Functional Union of Metal-Organic Complex and Chemically Complementary Surface ................................................................................. 5 Tobin Marks – Supported Organometallic Complexes: Surface Chemistry, Spectroscopy, Catalysis and Homogeneous Models ............................................ 8 Sunday Afternoon, Session II Susannah Scott – Exploring the Relationship between Homogeneous and Heterogeneous Reaction Kinetics .................................................................... 13 Justin Notestein – Templating Routes to Supported Oxide Catalysts by Design ..... 19 Liviu Mirica – Novel Palladium Catalysts for the Oxidative Oligomerization of Methane & Carbon
Recommended publications
  • The Progression of Chiral Anions from Concepts to Applications in Asymmetric Catalysis Robert J

    The Progression of Chiral Anions from Concepts to Applications in Asymmetric Catalysis Robert J

    REVIEW ARTICLE PUBLISHED ONLINE: 24 JULY 2012 | DOI: 10.1038/NCHEM.1405 The progression of chiral anions from concepts to applications in asymmetric catalysis Robert J. Phipps, Gregory L. Hamilton and F. Dean Toste* Despite the tremendous advances of the past four decades, chemists are far from being able to use chiral catalysts to con- trol the stereoselectivity of any desired reaction. New concepts for the construction and mode of operation of chiral catalysts have the potential to open up previously inaccessible reaction space. The recognition and categorization of distinct approaches seems to play a role in triggering rapid exploration of new territory. This Review both reflects on the origins as well as details a selection of the latest examples of an area that has advanced considerably within the past five years or so: the use of chiral anions in asymmetric catalysis. Defining reactions as involving chiral anions is a difficult task owing to uncertainties over the exact catalytic mechanisms. Nevertheless, we attempt to provide an overview of the breadth of reactions that could reasonably fall under this umbrella. 9 ithin the broader field of science, organic chemistry is Of significantly greater acidity (pKa around 2–4) are chiral phos- often referred to as a mature field of study. In spite of this, phoric acids, commonly derived from BINOL (1,1′-bi-2-naphthol). Wnew avenues of inquiry seem to arise with relative fre- These catalysts have risen to prominence over the past decade quency. Perhaps we take it for granted that expansions of the field because their high acidity permits activation of a broad range of are sparked when one or two chemical laboratories uncover a new substrates3,10.
  • Opportunities for Catalysis in the 21St Century

    Opportunities for Catalysis in the 21St Century

    Opportunities for Catalysis in The 21st Century A Report from the Basic Energy Sciences Advisory Committee BASIC ENERGY SCIENCES ADVISORY COMMITTEE SUBPANEL WORKSHOP REPORT Opportunities for Catalysis in the 21st Century May 14-16, 2002 Workshop Chair Professor J. M. White University of Texas Writing Group Chair Professor John Bercaw California Institute of Technology This page is intentionally left blank. Contents Executive Summary........................................................................................... v A Grand Challenge....................................................................................................... v The Present Opportunity .............................................................................................. v The Importance of Catalysis Science to DOE.............................................................. vi A Recommendation for Increased Federal Investment in Catalysis Research............. vi I. Introduction................................................................................................ 1 A. Background, Structure, and Organization of the Workshop .................................. 1 B. Recent Advances in Experimental and Theoretical Methods ................................ 1 C. The Grand Challenge ............................................................................................. 2 D. Enabling Approaches for Progress in Catalysis ..................................................... 3 E. Consensus Observations and Recommendations..................................................
  • Organic Chemistry

    Organic Chemistry

    Wisebridge Learning Systems Organic Chemistry Reaction Mechanisms Pocket-Book WLS www.wisebridgelearning.com © 2006 J S Wetzel LEARNING STRATEGIES CONTENTS ● The key to building intuition is to develop the habit ALKANES of asking how each particular mechanism reflects Thermal Cracking - Pyrolysis . 1 general principles. Look for the concepts behind Combustion . 1 the chemistry to make organic chemistry more co- Free Radical Halogenation. 2 herent and rewarding. ALKENES Electrophilic Addition of HX to Alkenes . 3 ● Acid Catalyzed Hydration of Alkenes . 4 Exothermic reactions tend to follow pathways Electrophilic Addition of Halogens to Alkenes . 5 where like charges can separate or where un- Halohydrin Formation . 6 like charges can come together. When reading Free Radical Addition of HX to Alkenes . 7 organic chemistry mechanisms, keep the elec- Catalytic Hydrogenation of Alkenes. 8 tronegativities of the elements and their valence Oxidation of Alkenes to Vicinal Diols. 9 electron configurations always in your mind. Try Oxidative Cleavage of Alkenes . 10 to nterpret electron movement in terms of energy Ozonolysis of Alkenes . 10 Allylic Halogenation . 11 to make the reactions easier to understand and Oxymercuration-Demercuration . 13 remember. Hydroboration of Alkenes . 14 ALKYNES ● For MCAT preparation, pay special attention to Electrophilic Addition of HX to Alkynes . 15 Hydration of Alkynes. 15 reactions where the product hinges on regio- Free Radical Addition of HX to Alkynes . 16 and stereo-selectivity and reactions involving Electrophilic Halogenation of Alkynes. 16 resonant intermediates, which are special favor- Hydroboration of Alkynes . 17 ites of the test-writers. Catalytic Hydrogenation of Alkynes. 17 Reduction of Alkynes with Alkali Metal/Ammonia . 18 Formation and Use of Acetylide Anion Nucleophiles .
  • The Selective Synthesis of Aromatics and Furans From

    The Selective Synthesis of Aromatics and Furans From

    THE SELECTIVE SYNTHESIS OF AROMATICS AND FURANS FROM BIOMASS-DERIVED COMPOUNDS by Eyas Mahmoud A dissertation submitted to the Faculty of the University of Delaware in partial fulfillment of the requirements for the degree of Doctor of Philosophy in Chemical Engineering Summer 2016 © 2016 Eyas Mahmoud All Rights Reserved THE SELECTIVE SYNTHESIS OF AROMATICS AND FURANS FROM BIOMASS-DERIVED COMPOUNDS by Eyas Mahmoud Approved: __________________________________________________________ Abraham M. Lenhoff, Ph.D. Chair of the Department of Chemical and Biomolecular Engineering Approved: __________________________________________________________ Babatunde A. Ogunnaike, Ph.D. Dean of the College of Engineering Approved: __________________________________________________________ Ann L. Ardis, Ph.D. Senior Vice Provost for Graduate and Professional Education I certify that I have read this dissertation and that in my opinion it meets the academic and professional standard required by the University as a dissertation for the degree of Doctor of Philosophy. Signed: __________________________________________________________ Raul F. Lobo, Ph.D. Professor in charge of dissertation I certify that I have read this dissertation and that in my opinion it meets the academic and professional standard required by the University as a dissertation for the degree of Doctor of Philosophy. Signed: __________________________________________________________ Dionisios G. Vlachos, Ph.D. Member of dissertation committee I certify that I have read this dissertation and that in my opinion it meets the academic and professional standard required by the University as a dissertation for the degree of Doctor of Philosophy. Signed: __________________________________________________________ Donald A. Watson, Ph.D. Member of dissertation committee I certify that I have read this dissertation and that in my opinion it meets the academic and professional standard required by the University as a dissertation for the degree of Doctor of Philosophy.
  • Surface Reactions and Chemical Bonding in Heterogeneous Catalysis

    Surface Reactions and Chemical Bonding in Heterogeneous Catalysis

    Surface reactions and chemical bonding in heterogeneous catalysis Henrik Öberg Doctoral Thesis in Chemical Physics at Stockholm University 2014 Thesis for the Degree of Doctor of Philosophy in Chemical Physics Department of Physics Stockholm University Stockholm 2014 c Henrik Oberg¨ ISBN 978-91-7447-893-8 Abstract This thesis summarizes studies which focus on addressing, using both theoretical and experimental methods, fundamental questions about surface phenomena, such as chemical reactions and bonding, related to processes in heterogeneous catalysis. The main focus is on the theoretical approach and this aspect of the results. The included articles are collected into three categories of which the first contains detailed studies of model systems in heterogeneous catalysis. For example, the trimerization of acetylene adsorbed on Cu(110) is measured using vibrational spectroscopy and modeled within the framework of Density Functional Theory (DFT) and quantitative agreement of the reaction barriers is obtained. In the second category, aspects of fuel cell catalysis are discussed. O2 dissociation is rate-limiting for the reduction of oxygen (ORR) under certain conditions and we find that adsorbate-adsorbate interactions are decisive when modeling this reaction step. Oxidation of Pt(111) (Pt is the electrocatalyst), which may alter the overall activity of the catalyst, is found to start via a PtO-like surface oxide while formation of a-PtO2 trilayers precedes bulk oxidation. When considering alternative catalyst materials for the ORR, their stability needs to be investigated in detail under realistic conditions. The Pt/Cu(111) skin alloy offers a promising candidate but segregation of Cu atoms to the surface is induced by O adsorption.
  • Surface Models in Heterogeneous Catalysis the Synthesis of Ammonia and the Conversion of Carbon Monoxide

    Surface Models in Heterogeneous Catalysis the Synthesis of Ammonia and the Conversion of Carbon Monoxide

    JOURNAL OF CATALYSIS 8, 29-35 (1967) Surface Models in Heterogeneous Catalysis The Synthesis of Ammonia and the Conversion of Carbon Monoxide G. PARRAVANO From the Deparzment qf Chemical and Metallurgical Engineering, University qf Michigan Ann Arbor, Machigan Received November 16, 1966, revised January 16, 1967 The establishment of chemical equilibria between gas and solid catalysts during the synthesis of NH3 and the conversion of CO is considered. Suitable solid-gas equilibrium reactions are discussed. With the correct choice of the rate-controlling step, the equilib- rium surface models are able to reproduce the experimental expressions for the rates of reaction. These models represent a drastic departure from the concept of a fixed, hetero- geneous surface that has been extensively used in the past for the interpretation of the experimental results on the above reactions. The two approaches, however, complement each other and the validity of each one may well be justified under different experimental conditions. Thus, a model may be considered the extension of the other by modification of some of the parameters of the system. Over the past several years many investi- view and it is certainly invalid for relatively gations have been carried out on the catalytic long periods of catalyst operation. It is, synthesis of NH3 and on the conversion of therefore, of interest to consider other CO. The studies have generally been directed possibilities more physically justifiable. toward the understanding of the nature, In this direction it seems particularly properties, and operation of the catalytic important to consider the possibility that surface through the analysis of experimental equilibration reactions between surface and results of reaction rates.
  • 1 the Structure and Reactivity of Single and Multiple

    1 the Structure and Reactivity of Single and Multiple

    1 1 The Structure and Reactivity of Single and Multiple Sites on Heterogeneous and Homogeneous Catalysts: Analogies, Differences, and Challenges for Characterization Methods Adriano Zecchina , Silvia Bordiga , and Elena Groppo 1.1 Introduction The content of this book is specifi cally devoted to a description of the complexity of the catalytic centers (both homogeneous and heterogeneous) viewed as nanoma- chines for molecular assembling. Although the word “ nano ” is nowadays some- what abused, its use for catalysts science (as nanoscience) is fully justifi ed. It is a matter of fact that (i) to perform any specifi c catalytic action, the selective catalyst must necessarily possess sophisticated structure where substrates bonds are broken and formed along a specifi c path and (ii) the relevant part of this structure, usually constituted by a metal center or metal cluster surrounded by a sphere of ligands or by a solid framework or by a portion of functionalized surface, often reaches the nanometric dimension. As it will emerge from the various chapters, this vision is valid for many types of selective catalysts including catalysts for hydrogenation, polymerization, olygomerization, partial oxidation, and photocata- lytic solar energy conversion. Five chapters are devoted to the above - mentioned reactions. From the point of view of the general defi nition, homogeneous and heterogeneous selective catalysts can be treated in the same way. As homogeneous selective catalysts are concerned, the tridimensional structure surrounding the metal center can be organized with cavitand shape, while for heterogeneous cata- lysts the selectivity is the result of an accurate design and synthesis of the frame- work structures (often microporous and crystalline) where the sites are anchored.
  • The Kinetics of Elementary Thermal Reactions in Heterogene- Ous Catalysis

    The Kinetics of Elementary Thermal Reactions in Heterogene- Ous Catalysis

    1 The kinetics of elementary thermal reactions in heterogene- 2 ous catalysis 3 G. Barratt Park1,2, Theofanis Kitsopoulos2,5,6, Dmitriy Borodin1, Kai Golibrzuch2, Jannis 4 Neugebohren1, Daniel J. Auerbach2, Charles T. Campbell4 & Alec M. Wodtke1,2,3* 5 1Institute for Physical Chemistry, Georg-August University of Goettingen, Tammannstraße 6, 6 37077 Göttingen, Germany. 7 2Department of Dynamics at Surfaces, Max Planck Institute for Biophysical Chemistry, Am 8 Faßberg 11, 37077 Göttingen, Germany. 9 3International Center for Advanced Studies of Energy Conversion, Georg-August University 10 of Goettingen, Tammannstraße 6, 37077 Göttingen, Germany. 11 4 Department of Chemistry, University of Washington, Seattle, WA 98195-1700, USA 12 5 Department of Chemistry, University of Crete, Heraklion, Greece 13 6 Institute of Electronic Structure and Laser – FORTH, Heraklion, Greece 14 15 *email: [email protected] 16 17 KEYWORDS: Ion-imaging, velocity-resolved kinetics, CO oxidation, heterogeneous catalysis, 18 slice ion-imaging, molecular beams, surface chemistry. 19 20 1 21 Abstract 22 The kinetics of elementary reactions is fundamental to our understanding of catalysis. Just as 23 micro-kinetic models of atmospheric chemistry provided the predictive power that led to the 24 Montreal protocol reversing loss of stratospheric ozone, pursuing a micro-kinetic approach to 25 heterogeneous catalysis has tremendous potential for societal impact. However, developing this 26 approach for catalysis faces great challenges. Methods for measuring rate constants are quite 27 limited and present predictive theoretical methods remain largely un-validated. This paper pre- 28 sents a short perspective on recent experimental advances in our ability to measure the rates of 29 elementary reactions at surfaces that rely on a stroboscopic pump-probe concept for neutral 30 matter.
  • Water Splitting by Heterogeneous Catalysis

    Water Splitting by Heterogeneous Catalysis

    !"#$ #"%"" &' () * ( +# ,% - . ( (.( ( . %/ .0! 1 ( % 2 3 . 4 . 5 % . . % . . . . . . 3 % !# 3 ( 3 ( 3 ( 3 %/. . - % . (. 6 7 % ( 2!0! . (/ (3 . 7 % ( ( 3 % . 3 ( %/ . 8 9 3 8 % ( :;0 9 . <= 3 9 . % ( . ( 3 > % !"#$ ?@@ %% @ A B ?? ? ? #;C#C# ,8D$CD#$$D$":D! ,8D$CD#$$D$";"C ! " # $ (#" D# WATER SPLITTING BY HETEROGENEOUS CATALYSIS Henrik Svengren Water splitting by heterogeneous catalysis Henrik Svengren ©Henrik Svengren, Stockholm University 2017 ISBN print 978-91-7797-039-2 ISBN PDF 978-91-7797-040-8 Printed in Sweden by Universitetsservice US-AB, Stockholm 2017 Distributed by the Department of Materials and Environmental Chemistry To my beloved family Cover image + Heterogeneous catalysis of water oxidation according to 2H2O ĺ O2 + 4H on CoSbO4/CoSb2O6, investigated in Paper II. The figure is composed of SEM- and TEM images, structural drawings, reactant- and product molecules. i Examination Faculty opponent Docent Tomas Edvinsson Solid State Physics Department of Engineering Sciences Uppsala University,
  • Synthesis, Catalysis, and Chemistry

    Synthesis, Catalysis, and Chemistry

    University of Massachusetts Amherst ScholarWorks@UMass Amherst Doctoral Dissertations Dissertations and Theses July 2017 Nanoporous Solid Acid Materials for Biomass Conversion into Value-Added Chemicals: Synthesis, Catalysis, and Chemistry Hong Je Cho University of Massachusetts Amherst Follow this and additional works at: https://scholarworks.umass.edu/dissertations_2 Part of the Catalysis and Reaction Engineering Commons Recommended Citation Cho, Hong Je, "Nanoporous Solid Acid Materials for Biomass Conversion into Value-Added Chemicals: Synthesis, Catalysis, and Chemistry" (2017). Doctoral Dissertations. 952. https://doi.org/10.7275/9584937.0 https://scholarworks.umass.edu/dissertations_2/952 This Open Access Dissertation is brought to you for free and open access by the Dissertations and Theses at ScholarWorks@UMass Amherst. It has been accepted for inclusion in Doctoral Dissertations by an authorized administrator of ScholarWorks@UMass Amherst. For more information, please contact [email protected]. NANOPOROUS SOLID ACID MATERIALS FOR BIOMASS CONVERSION INTO VALUE-ADDED CHEMICALS: SYNTHESIS, CATALYSIS, AND CHEMISTRY A Dissertation Presented by HONG JE CHO Submitted to the Graduate School of the University of Massachusetts Amherst in partial fulfillment of the requirements for the degree of DOCTOR OF PHILOSOPHY May 2017 Chemical Engineering © Copyright by Hong Je Cho 2017 All Rights Reserved NANOPOROUS SOLID ACID MATERIALS FOR BIOMASS CONVERSION INTO VALUE-ADDED CHEMICALS: SYNTHESIS, CATALYSIS, AND CHEMISTRY A Dissertation Presented by HONG JE CHO Approve as to style and content by: ______________________________________ Wei Fan, Chair ______________________________________ Friederike Jentoft, Member ______________________________________ Ashwin Ramasubramaniam, Member ___________________________________ John Klier, Department Head Department of Chemical Engineering ACKNOWLEDGEMENTS This work was supported by Catalysis Center for Energy Innovation (funded by the US Dept.
  • Catalysis and Reaction Engineering Division 2020

    Catalysis and Reaction Engineering Division 2020

    Catalysis and Reaction Engineering Division 2020 Held at the 2020 AIChE Annual Meeting Online 16 – 20 November 2020 Volume 1 of 2 ISBN: 978-1-7138-2313-1 Printed from e-media with permission by: Curran Associates, Inc. 57 Morehouse Lane Red Hook, NY 12571 Some format issues inherent in the e-media version may also appear in this print version. Copyright© (2020) by AIChE All rights reserved. Printed with permission by Curran Associates, Inc. (2021) For permission requests, please contact AIChE at the address below. AIChE 120 Wall Street, FL 23 New York, NY 10005-4020 Phone: (800) 242-4363 Fax: (203) 775-5177 www.aiche.org Additional copies of this publication are available from: Curran Associates, Inc. 57 Morehouse Lane Red Hook, NY 12571 USA Phone: 845-758-0400 Fax: 845-758-2633 Email: [email protected] Web: www.proceedings.com TABLE OF CONTENTS VOLUME 1 (19A) CATALYTIC REACTION PATHWAYS AND PROCESS SYNTHESIS FOR BIOMASS CONVERSION TO HIGH-VALUE CHEMICALS FOR ORGANIC DYE AND POLYMER APPLICATIONS .................................................................................................................................................. 1 Hochan Chang, Ishan Bajaj, George W. Huber, Christos T. Maravelias, James A. Dumesic (19B) SUPERACID POLYMER CATALYSTS FOR HYDROXYMETHYLFURFURAL PRODUCTION .................................................................................................................................................... 2 Ibeh S. Omodolor, Sarah A. Walz, Subhash Kalidindi, Vimantha Bamunuarachchi, Ravikumar Gogar,
  • Catalytic Oxidation of NO to NO2 for Nitric Acid Production Over a Pt

    Catalytic Oxidation of NO to NO2 for Nitric Acid Production Over a Pt

    1 Catalytic oxidation of NO to NO2 for nitric acid production over a Pt/Al2O3 catalyst Ata ul Rauf Salmana, Bjørn Christian Engerb, Xavier Auvraya c, Rune Lødengb, Mohan Menond, David Wallerd, Magnus Rønninga* a Department of Chemical Engineering, Norwegian University of Science and Technology (NTNU), Sem Sælands vei 4, NO-7491 Trondheim, Norway. b SINTEF Industry, Kinetic and Catalysis group, P.O. Box 4760 Torgarden, NO-7465 Trondheim, Norway. c Current address: Competence Centre for Catalysis, Chemical Engineering, Chalmers University of Technology, S-412 96 Gothenburg, Sweden d YARA Technology Center, Herøya Forskningspark, Bygg 92, Hydrovegen 67, NO-3936 Porsgrunn, Norway. * Corresponding author. Tel.: +47 73594121. E-mail address: [email protected] (M. Rønning). 2 Abstract The oxidation of nitric oxide (NO) to nitrogen dioxide (NO2) is a key step both in NOx abatement technologies as well as in the Ostwald process for nitric acid production. A 1 wt.% Pt/Al2O3 catalyst was used to study oxidation of nitric oxide at two different concentrations of NO; 400 ppm NO (representative of engine exhaust treatment) and 10% NO (nitric acid plant). The catalyst was characterised using N2 adsorption and CO chemisorption. The effect of temperature and feed concentration on catalytic activity was investigated. For a feed comprising of 10% NO and 6% O2, Pt/Al2O3 exhibits significant catalytic activity above o 300 C. Addition of 15% H2O in the feed had an insignificant effect on activity of the catalyst. We report for the first time the kinetics for oxidation of NO to NO2 under nitric acid plant conditions. An apparent activation energy of 33 kJ/mol was observed.