Engineering and. Tapio Salmi Abo Akademi Abo-Turku, Finland. Jyri-Pekka Mikkola. Umea University, Umea, Sweden. Johan Warna.

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1 Chemical Reaction Engineering and Reactor Technology Tapio Salmi Abo Akademi Abo-Turku, Finland Jyri-Pekka Mikkola Umea University, Umea, Sweden Johan Warna Abo Akademi Abo-Turku, Finland CRC Press is CRC Press Taylor &. Francis Croup Boca Raton London New York an imprint of the Taylor & Francis Group, an Informa business

2 Contents Preface xix Notations xxiii Chapter 1 Introduction PRELIMINARY STUDIES Reaction Stoichiometry, Thermodynamics, and Synthesis Routes LABORATORY EXPERIMENTS ANALYSIS OF THE EXPERIMENTAL RESULTS SIMULATION OF REACTOR MODELS INSTALLATION OF A PILOT-PLANT UNIT CONSTRUCTION OF THE FACILITY IN FULL SCALE 6 REFERENCES 7 Chapter 2 Stoichiometry and Kinetics STOICHIOMETRIC MATRIX REACTION KINETICS Elementary Reactions Kinetics of Nonelementary Reactions: Quasi-Steady- State and Quasi-Equilibrium Approximations Ionic and Radical Intermediates 18 xi

3 xii Contents Catalytic Processes: Eley-Rideal Mechanism Catalytic Processes: Langmuir-Hinshelwood Mechanism 24 REFERENCES 25 Chapter 3 Homogeneous Reactors REACTORS FOR HOMOGENEOUS REACTIONS HOMOGENEOUS TUBE REACTOR WITH A PLUG FLOW Mass Balance Energy Balance HOMOGENEOUS TANK REACTOR WITH PERFECT MIXING Mass Balance Energy Balance HOMOGENEOUS BR Mass Balance Energy Balance MOLAR AMOUNT, MOLE FRACTION, REACTION EXTENT, CONVERSION, AND CONCENTRATION Definitions Relation between Molar Amount, Extent of Reaction, Conversion, and Molar Fraction A System with a Single Chemical Reaction A System with Multiple Chemical Reactions Relationship between Concentration, Extent of Reaction, Conversion, and Volumetric Flow Rate in a Continuous Reactor Gas-Phase Reactions Liquid-Phase Reactions Relationship between Concentration, Extent of Reaction, Conversion, and Total Pressure in a BR Gas-Phase Reactions Liquid-Phase Reactions STOICHIOMETRY IN MASS BALANCES EQUILIBRIUM REACTOR: ADIABATIC TEMPERATURE CHANGE Mass and Energy Balances ANALYTICAL SOLUTIONS FOR MASS AND ENERGY BALANCES Multiple Reactions First-Order Parallel Reactions Momentaneous and Integral Yield for Parallel Reactions Reactor Selection and Operating Conditions for Parallel Reactions First-Order Consecutive Reactions Consecutive-Competitive Reactions Product Distributions in PFRs and BRs 84

4 Contents a xiii Product Distribution in a CSTR Comparison ofideal Reactors NUMERICAL SOLUTION OF MASS BALANCES FOR VARIOUS COUPLED REACTIONS 89 REFERENCES 92 Chapter 4 Nonideal Reactors: Residence Time Distributions RESIDENCE TIME DISTRIBUTION IN FLOW REACTORS Residence Time as a Concept Methods for Determining RTDs Volume Element Tracer Experiments RESIDENCE TIME FUNCTIONS Population Density Function E( Distribution Functions F(t) and F*(t) Intensity Function Mf) Mean Residence Time C Function Dimensionless Time Variance Experimental Determination of Residence Time Functions RTD for a CSTR and PFR RTD in Tube Reactors with a Laminar Flow SEGREGATION AND MAXIMUM MIXEDNESS Segregation Model Maximum Mixedness Model TANKS-IN-SERIES MODEL Residence Time Functions for the Tanks-in-Series Model Tanks in Series as a Chemical Reactor Maximum-Mixed Tanks-in-Series Model Segregated Tanks in Series Comparison of Tanks-in-Series Models Existence of Micro- and Macrofluids AXIAL DISPERSION MODEL RTDs for the Axial Dispersion Model Axial Dispersion Model as a Chemical Reactor Estimation of the Axial Dispersion Coefficient TUBE REACTOR WITH A LAMINAR FLOW Laminar Reactor without Radial Diffusion Laminar Reactor with a Radial Diffusion: Axial Dispersion Model 13 7 REFERENCES 139

5 xiv Contents Chapter 5 Catalytic Two-Phase Reactors REACTORS FOR HETEROGENEOUS CATALYTIC GAS- AND LIQUID-PHASE REACTIONS PACKED BED Mass Balances for the One-Dimensional Model Effectiveness Factor Chemical Reaction and Diffusion inside a Catalyst Particle Spherical Particle Slab Asymptotic Effectiveness Factors for Arbitrary Kinetics Nonisothennal Conditions Energy Balances for the One-Dimensional Model Mass and Energy Balances for the Two-Dimensional Model Pressure Drop in Packed Beds FLUIDIZED BED Mass Balances According to Ideal Models Kunii-Levenspiel Model for Fluidized Beds J Kunii-Levmspiel Parameters PARAMETERS FOR PACKED BED AND FLUIDIZED BED REACTORS 210 REFERENCES 212 Chapter 6 Catalytic Three-Phase Reactors REACTORS USED FOR CATALYTIC THREE-PHASE REACTIONS MASS BALANCES FOR THREE-PHASE REACTORS Mass Transfer and Chemical Reaction Three-Phase Reactors with a Plug Flow Three-Phase Reactor with Complete Backmixing Semibatch and BRs Parameters in Mass Balance Equations ENERGY BALANCES FOR THREE-PHASE REACTORS Three-Phase PFR Tank Reactor with Complete Backmixing Batch Reactor Analytical and Numerical Solutions of Balance Equations for Three-Phase Reactors Sulfur Dioxide Oxidation Hydrogenation ofawmatics Carbonyl Group Hydrogenation 242 REFERENCES 244

6 Contents xv Chapter 7 Gas-Liquid Reactors REACTORS FOR NONCATALYTIC AND HOMOGENEOUSLY CATALYZED REACTIONS MASS BALANCES FOR IDEAL GAS-LIQUID REACTORS Plug Flow Column Reactor Tank Reactor with Complete Backmixing Batch Reactor Fluxes in Gas and Liquid Films Very Slow Reactions Slow Reactions Reactions with a Finite Velocity Fluxes in Reactor Mass Balances Design of Absorption Gas and Liquid Film Coefficients, Diffusion Coefficients, and Columns 284 Gas-Liquid Equilibria ENERGY BALANCES FOR GAS-LIQUID REACTORS Plug Flow Column Reactor Tank Reactor with Complete Backmixing Batch Reactor Coupling of Mass and Energy Balances Numerical Solution of Gas-Liquid Reactor Balances 293 REFERENCES 295 Chapter 8 Reactors for Reactive Solids REACTORS FOR PROCESSES WITH REACTIVE SOLIDS MODELS FOR REACTIVE SOLID PARTICLES Definitions Product Layer Model First-Order Reactions General Reaction Kinetics: Diffusion Resistance as the Rate-Determining Step Shrinking Particle Model First-Order Reactions Arbitrary Reaction Kinetics: Diffusion Resistance in the Gas Film as the Rate-Determining Step MASS BALANCES FOR REACTORS CONTAINING A SOLID REACTIVE PHASE Batch Reactor Particles with a Porous Product Layer Shrinking Particles Semibatch Reactor Particle with a Porous Product Layer 322

7 xvi Contents Shrinking Particle Packed Bed 322 REFERENCES 325 Chapter 9 Toward New Reactor and Reaction Engineering HOW TO APPROACH THE MODELING OF NOVEL REACTOR CONCEPTS? REACTOR STRUCTURES AND OPERATION MODES Reactors with Catalyst Packings Mass Balances for the Gas and Liquid Bulk Phases Intel-facial Transport Mass Balances for the Catalyst Particles Numerical Solution ofthe Column Reactor Model Concluding Summary Monolith Reactors Flow Distribution from CFD Calculations Simplified Model for Reactive Flow Application: Catalytic Three-Phase Hydrogenation of Citral in the Monolith Reactor Fiber Reactor Membrane Reactor Microreactor TRANSIENT OPERATION MODES AND DYNAMIC MODELING Periodic Switching of Feed Composition Reverse Flow Reactors NOVEL FORMS OF ENERGY AND REACTION MEDIA Ultrasound Microwaves Supercritical Fluids Case: Hydrogenation of Triglycerides Ionic Liquids Case: Heterogenized ILs as Catalysis EXPLORING REACTION ENGINEERING FOR NEW APPLICATIONS Case Study: Delignification of Wood SUMMARY 370 REFERENCES 371 Chapter 10 Chemical Reaction Engineering: Historical Remarks and Future Challenges CHEMICAL REACTION ENGINEERING AS A PART OF CHEMICAL ENGINEERING EARLY ACHIEVEMENTS OF CHEMICAL ENGINEERING 374

8 Contents xvii 10.3 THE ROOTS OF CHEMICAL REACTION ENGINEERING UNDERSTANDING CONTINUOUS REACTORS AND TRANSPORT PHENOMENA POSTWAR TIME: NEW THEORIES EMERGE NUMERICAL MATHEMATICS AND COMPUTING DEVELOP TEACHING THE NEXT GENERATION EXPANSION OF CHEMICAL REACTION ENGINEERING: TOWARD NEW PARADIGMS 380 FURTHER READING 382 Chapter 11 Exercises 383 Chapter 12 Solutions of Selected Exercises 445 Appendix 1 Solutions of Algebraic Equation Systems 535 Appendix 2 Solutions of ODEs 537 A2.1 SEMI-IMPLICIT RUNGE-KUTTA METHOD 537 A2.2 LINEAR MULTISTEP METHODS 539 REFERENCES 541 Appendix 3 Computer Code NLEODE 543 A3.1 SUBROUTINE FCN 544 A3.2 SUBROUTINE FCNJ 544 REFERENCES 547 Appendix 4 Gas-Phase Diffusion Coefficients 549 REFERENCE 552 Appendix 5 Fluid-Film Coefficients 553 A5.1 GAS-SOLID COEFFICIENTS 553 A5.2 GAS-LIQUID AND LIQUID-SOLID COEFFICIENTS 554 REFERENCES 555 Appendix 6 Liquid-Phase Diffusion Coefficients 557 A6.1 NEUTRAL MOLECULES 557 A6.2 IONS 558 REFERENCES 562

9 xviii Contents Appendix 7 Correlations for Gas-Liquid Systems 563 A7.1 BUBBLE COLUMNS 563 A7.2 PACKED COLUMNS 565 A7.3 SYMBOLS 567 A7.4 INDEX 568 A7.5 DIMENSIONLESS NUMBERS 568 REFERENCES 568 Appendix 8 Gas Solubilities 569 REFERENCES 572 Appendix 9 Laboratory Reactors 573 A9.1 FLOW PATTERN IN LABORATORY REACTORS 573 A9.2 MASS TRANSFER RESISTANCE 574 A9.3 HOMOGENEOUS BR 575 A9.4 HOMOGENEOUS STIRRED TANK REACTOR 577 A9.5 FIXED BED IN THE INTEGRAL MODE 578 A9.6 DIFFERENTIAL REACTOR 579 A9.7 GRADIENTLESS REACTOR 581 A9.8 BRs FOR TWO- AND THREE-PHASE PROCESSES 582 A9.9 CLASSIFICATION OF LABORATORY REACTOR MODELS 584 REFERENCES 585 Appendix 10 Estimation of Kinetic Parameters from Experimental Data 587 A10.1 COLLECTION OF KINETIC DATA 587 A10.2 INTEGRAL METHOD 590 A10.3 DIFFERENTIAL METHOD 594 A10.4 RECOMMENDATIONS 596 A10.5 INTRODUCTION TO NONLINEAR REGRESSION 596 A10.6 GENERAL APPROACH TO NONLINEAR REGRESSION IN CHEMICAL REACTION ENGINEERING 598 REFERENCES 604 Author Index 605 Subject Index 607

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