Modeling and Simulation of Heterogeneous Catalytic Reactions: From the Molecular Process to the Technical System

The Nobel Prize in Chemistry 2007 awarded to Gerhard Ertl for his groundbreaking studies in surface chemistry highlighted the importance of heterogeneous catalysis not only for modern chemical industry but also for environmental protection. Heterogeneous catalysis is seen as one of the key technologies which could solve the challenges associated with the increasing diversification of raw materials and energy sources. It is the decisive step in most chemical industry processes, a major method of reducing pollutant emissions from mobile sources and is present in fuel cells to produce electricity. The increasing power of computers over the last decades has led to modeling and numerical simulation becoming valuable tools in heterogeneous catalysis. This book covers many aspects, from the state-of-the-art in modeling and simulations of heterogeneous catalytic reactions on a molecular level to heterogeneous catalytic reactions from an engineering perspective. This first book on the topic conveys expert knowledge from surface science to both chemists and engineers interested in heterogeneous catalysis. The well-known and international authors comprehensively present many aspects of the wide bridge between surface science and catalytic technologies, including DFT calculations, reaction dynamics on surfaces, Monte Carlo simulations, heterogeneous reaction rates, reactions in porous media, electro-catalytic reactions, technical reactors, and perspectives of chemical and automobile industry on modeling heterogeneous catalysis. The result is a one-stop reference for theoretical and physical chemists, catalysis researchers, materials scientists, chemical engineers, and chemists in industry who would like to broaden their horizon and get a substantial overview on the different aspects of modeling and simulation of heterogeneous catalytic reactions.

Table of Contents:
Preface MODELING CATALYTIC REACTIONS ON SURFACES WITH DENSITY FUNCTIONAL THEORY Introduction Theoretical Background The Electrocatalytic Oxygen Reduction Reaction on Pt(111) Conclusions DYNAMICS OF REACTIONS AT SURFACES Introduction Theoretical and Computational Foundations of Dynamical Simulations Interpolation of Potential Energy Surfaces Quantum Dynamics of Reactions at Surfaces Nondissociative Molecular Adsorption Dynamics Adsorption Dynamics on Precovered Surfaces Relaxation Dynamics of Dissociated H2 Molecules Electronically Nonadiabatic Reaction Dynamics Conclusions FIRST-PRINCIPLES KINETIC MONTE CARLO SIMULATIONS FOR HETEROGENEOUS CATALYSIS: CONCEPTS, STATUS, AND FRONTIERS Introduction Concepts and Methodology A Showcase Frontiers Conclusions MODELING THE RATE OF HETEROGENEOUS REACTIONS Introduction Modeling the Rates of Chemical Reactions in the Gas Phase Computation of Surface Reaction Rates on a Molecular Basis Models Applicable for Numerical Simulation of Technical Catalytic Reactors Simplifying Complex Kinetic Schemes Summary and Outlook MODELING REACTIONS IN POROUS MEDIA Introduction Modeling Porous Structures and Surface Roughness Diffusion Diffusion and Reaction Pore Structure Optimization: Synthesis Conclusion MODELING POROUS MEDIA TRANSPORT, HETEROGENEOUS THERMAL CHEMISTRY, AND ELECTROCHEMICAL CHARGE TRANSFER Introduction Qualitative Illustration Gas-Phase Conservation Equations Ion and Electron Transport Charge Conservation Thermal Energy Chemical Kinetics Computational Algorithm Button Cell Example Summary and Conclusions EVALUATION OF MODELS FOR HETEROGENEOUS CATALYSIS Introduction Surface and Gas-Phase Diagnostic Methods Evaluation of Hetero/Homogeneous Chemical Reaction Schemes Evaluation of Transport Conclusions COMPUTATIONAL FLUID DYNAMICS OF CATALYTIC REACTORS Introduction Modeling of Reactive Flows Coupling of the Flow Field with Heterogeneous Chemical Reactions Numerical Methods and Computational Tools Reactor Simulations Summary and Outlook PERSPECTIVE OF INDUSTRY ON MODELING CATALYSIS The Industrial Challenge The Dual Approach The Role of Modeling Examples of Modeling and Scale-Up of Industrial Processes Conclusions PERSPECTIVES OF THE AUTOMOTIVE INDUSTRY ON THE MODELING OF EXHAUST GAS AFTERTREATMENT CATALYSTS Introduction Emission Legislation Exhaust Gas Aftertreatment Technologies Modeling of Catalytic Monoliths Modeling of Diesel Particulate Filters Selective Catalytic Reduction by NH3 (Urea-SCR) Modeling Diesel Oxidation Catalyst, Three-Way Catalyst, and NOx Storage and Reduction Catalyst Modeling Modeling Catalytic Effects in Diesel Particulate Filters Determination of Global Kinetic Parameters Challenges for Global Kinetic Models System Modeling of Combined Exhaust Aftertreatment Systems Conclusion

About the Author :
Olaf Deutschmann studied physics in Magdeburg and Berlin. In 1996, he obtained his doctoral degree (chemistry) from Heidelberg University supervised by Jurgen Warnatz. He then worked on high-temperature catalysis at the University of Minnesota with Lanny D. Schmidt and at the Los Alamos National Laboratory. After receiving the venia legendi in Physical Chemistry at Heidelberg University he joined the University of Karlsruhe in 2003. Today, he holds the Chair in Chemical Technology at the Karlsruhe Institute of Technology (KIT), Germany, and is speaker of the Helmholtz Research School Energy-Related Catalysis. His group works on heterogeneous reactions for the synthesis of chemicals and materials, reduction of pollutant emissions, and energy conversion. He is recipient of the DECHEMA Award of the Max Buchner Research Foundation and of the Hermann-Oberth-Medal in Silver.

Review :
“Overall the book is a good attempt to tackle a research topic that is very current. Indeed the book is up-to-date and there are very recent citations, many of which concern pgm applications in catalysis. In summary the book is a good introduction to the rapidly changing and wide reaching field of multiscale computational research.”  (Platinum Metals Review, 2012)