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Spatially Resolved Operando Measurements in Heterogeneous Catalytic Reactors

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Contents

Contributors

Preface

Chapter One: Understanding the Performance of Automotive Catalysts via Spatial Resolution of Reactions Inside Honeycomb M ...

1. Introduction

2. SpaciMS Methods

3. LNT Applications

3.1. NOx Storage and Regeneration

3.2. Regeneration With CO

3.3. Direct H2 vs Indirect Intermediate-NH3 Regeneration Pathways

3.4. Sulfation and Desulfation

3.5. LNT Modeling Using Spatiotemporal Data

3.6. Non-SpaciMS Methods for Resolving Distributed Intracatalyst Performance

4. SCR Applications

4.1. NOx and NH3 Reaction Distributions

4.2. Distributed NH3 Capacity Utilization

4.3. Operando NH3 Isotherms

4.4. SCR Modeling Using Spatiotemporal Data

4.5. Other Intracatalyst Distributed Measurements and Applications

5. Oxidation Catalyst Applications

6. Particulate Filter Applications

7. Summary and Conclusions

Acknowledgments

References

Chapter Two: Spatio-Temporal Phenomena in Monolithic Reactors Measured by Combined Spatially-Resolved Mass Spectrometry a ...

1. Introduction

2. Spatially Resolved Temperature Measurements

2.1. Review of Spatiotemporal Temperature Measurements

2.2. Optical Backscatter Reflectometer

2.2.1. Measurement of Spatiotemporal Temperature by c-OFDR

2.2.2. Theory

2.2.2.1. Optical Fiber Structure and Light Transmission Features

2.2.2.2. Reflected Spectral Scatter in the Optical Fiber

2.2.3. Coherent c-OFDR

2.2.4. Calibration and Testing Procedure for c-OFDR 4600 System

2.2.4.1. Calibration of the c-OFDR 4600 System

2.2.4.2. Spatial Temperature Measurement Testing

2.2.4.3. Practical Considerations of c-OFDR Operation

2.3. Applications of c-OFDR

2.3.1. Steady-State Spatial Temperature Profile of a Catalytic Exothermic Reaction

2.3.2. Spatiotemporal Temperature Measurements of Wrong-Way Behavior

3. Spatiotemporal Temperature and Concentration Measurement by c-OFDR and SpaciMS

3.1. Spatial Concentration Measurement by SpaciMS

3.2. Combined Spatiotemporal Measurements by SpaciMS and c-OFDR

3.2.1. Combined Steady-State Concentration and Temperature Measurements

3.3. Applications

3.3.1. Invasiveness of SpaciMS Measurements

3.3.2. Spatiotemporal Features of Lean/Rich Cycling

3.3.3. Spatiotemporal Features of the Catalytic Hydrocarbon Trap

3.3.3.1. Temperature Programmed Oxidation (TPO)

3.3.3.2. Spatially Resolved Hydrocarbon Trapping

3.3.3.3. Spatially Resolved TPO

3.3.3.4. Spatial Features of Oscillating Trapping and Oxidation

3.3.3.5. Mechanism of Multiple Hydrocarbon Light-Off During TPO

4. Conclusions

Acknowledgment

References

Further Reading

Chapter Three: In Situ Spatially Resolved Techniques for the Investigation of Packed Bed Catalytic Reactors: Current Stat ...

1. Introduction

2. Spatially Resolved Characterization Techniques for Fixed Beds

2.1. Spatially Resolved Spectroscopy for Fixed Beds

2.2. Spatial Resolution of Fixed Catalyst Beds Using Physical Probes

2.3. First-Generation Spaci-FB

2.4. Second-Generation Spaci-FB

2.5. Coupling Second-Generation Spaci-FB With XAS

3. Conclusions and Perspective on the Future of Spatially Resolved Techniques for Packed Bed Catalytic Reactors

Acknowledgments

References

Chapter Four: Analysis of the Impact of Gas-Phase Chemistry in Adiabatic CPO Reactors by Axially Resolved Measurements

1. Introduction

2. Application of the Spatially Resolved Sampling Technique to the CPO of C2+ Hydrocarbons

2.1. Experimental Methods

2.1.1. Catalyst

2.1.2. Apparatus and Operating Conditions

2.2. Mathematical Model of the Reactor and Kinetic Scheme

2.3. Detection of Gas-Phase Products in the Autothermal CPO of Propane

2.4. Effect of Pressure in the Autothermal CPO of Propane

2.4.1. Effect of Pressure up to 4bar

2.4.2. Effect of Pressure Above 4bar

2.5. Gas-Phase Chemistry in the Autothermal CPO of Octane Isomers

3. Role of Homogeneous Chemistry in Other Fuel-Rich Oxidation Processes

3.1. ODH of Ethane Over Pt and Rh

3.2. Oxidative Coupling of Methane

3.3. Partial Oxidation of Ethanol

4. Conclusions

References

Chapter Five: Imaging Gas Flow in Gas-Solid Catalytic Systems by Near-Infrared Tomography

1. Introduction

2. Speciation in Reactors by 2D Optical NIR Imaging Technique

2.1. Introduction to NIR Imaging

2.2. Application of 2D NIR Imaging to Catalyst Activity and Fluid Flow Inside Gas-Solid Catalytic Reactors

2.2.1. High-Throughput Screening of Catalyst Activity by NIR Imaging

3. Speciation in Reactors by Optical 3D Imaging Technique

3.1. 3D Distribution in Chemical Systems by Process Tomography

3.2. Transmittance Optical Tomography Through Nonopaque Media

3.3. Diffused Transmittance Optical Tomography Through Semiopaque Media

3.3.1. Application of Diffused Transmittance NIR Tomography to Packed bed Adsorbers

3.3.1.1. Experimental Setup and Validation

3.3.1.2. Flow Visualization and Temperature Measurement in a Packed Bed Adsorber of Low AR

3.3.2. Spatial Distributions of Composition and Temperature in Gas-Solid Packed Beds Reactor by NIR Tomography

3.3.3. Dispersion Profiles in Gas-Solid Packed Beds by NIR Tomography

3.3.3.1. Mass Dispersion Profiles by Spatially Resolved NIR Imaging

3.3.3.2. Mass Dispersion Profiles by DEM Modeling

3.3.4. Local Catalyst Activity Profiles in Gas-Solid Packed Beds by NIR Tomography

3.3.4.1. PROX of Carbon Monoxide

3.3.4.2. Local Deactivation Profiles by NIR Tomography

3.3.4.3. Results

3.3.4.3.1. Kinetics of PROX of CO

3.3.4.3.2. Local Deactivation Profiles by 2D and 3D Modeling

3.3.4.3.2.1. Analysis of Catalyst Deactivation in 2D Packed Bed Reactors of Low AR

3.3.4.3.2.2. Analysis of Catalyst Deactivation in 3D Packed Bed Reactors of Low AR

4. Conclusions

References

Index

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