Chemical Valorisation of Carbon Dioxide 1st Edition by Georgios Stefanidis, Andrzej Stankiewicz ISBN 9781839164071 1839164077

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ISBN 10: 1839164077
ISBN 13: 9781839164071
Author: Georgios Stefanidis, Andrzej Stankiewicz

The role of carbon dioxide in our changing climate is now hard to ignore, and many countries are making pledges to reduce or eliminate their carbon output. Chemical valorisation of carbon dioxide, as an alternative to sequestration, is likely to play an important part in reaching these targets, and as such is one of the fastest developing areas of green chemistry and chemical reaction engineering.

Providing a comprehensive panorama of recent advances in the methods and technologies for chemical valorisation of carbon dioxide, this book is essential reading for anyone with an interest in sustainability and green chemistry. Both the technological improvements in traditional processes and new methods and concepts are discussed, including various (renewable) electricity-based methods, as well as novel catalytic, photocatalytic and biocatalytic approaches

Chemical Valorisation of Carbon Dioxide 1st Edition Table of contents:

Chapter 1 – Turning CO2 into Fuels and Chemicals: An Introduction

1.1 Introduction

1.2 Role of CO2 to Chemicals and Fuels Paths in a Future Sustainable Scenario

1.2.1 How to Account for the Impact of CO2 Utilization

1.2.2 Putting CO2 Conversion to Chemicals and Fuels in the Right Scenario

1.2.3 The Cost of CO2 Conversion Technologies

1.3 Paths in CO2 to Chemicals and Fuels Conversion

1.4 Conclusions

List of Abbreviations

Acknowledgements

References

Chapter 2 – Carboxylation with CO2

2.1 Introduction

2.2 Carboxylation of Unsaturated Hydrocarbons via the Addition of Organometallic Species

2.2.1 Alkynes

2.2.2 Alkenes

2.2.3 Dienes

2.3 Oxidative Cyclization

2.3.1 Alkynes

2.3.2 Alkenes

2.3.3 Dienes

2.4 Carboxylation of Organometallic Reagents

2.4.1 Organoboron Compounds

2.4.2 Organozinc Compounds

2.4.3 Other Organometallic Reagents

2.5 Carboxylation of C–X Bonds

2.5.1 Aryl Halides

2.5.2 Alkyl Halides

2.5.3 Allylic Alcohols and Their Derivatives

2.6 Carboxylation of C–H Bonds

2.6.1 Carboxylation of C(sp)–H Bonds

2.6.2 Carboxylation of C(sp2)–H Bonds

2.6.3 Carboxylation of C(sp3)–H Bonds

2.7 Conclusions

References

Chapter 3 – Carbonylation with CO2

3.1 Carbonylation with CO2 to Generate Lactams

3.2 Carbonylation with CO2 to Generate Lactones

3.3 Carbonylation with CO2 to Generate Ketones

3.4 Carbonylation with CO2 to Generate Two Carbon–Heteroatom Bonds

3.5 Mass Transfer of Carbon Dioxide in Carbonylation Reaction

3.6 Conclusion

Acknowledgements

References

Chapter 4 – Modern Urea Synthesis

4.1 Introduction

4.2 Urea

4.2.1 A Comparison of Different Urea Production Technologies

4.3 Sustainable Urea Production by Employing the Theory of Change

4.3.1 A Comparison of Different Sustainable Hydrogen and Ammonia Production Processes

4.4 Conclusions

List of Abbreviations

Acknowledgements

References

Chapter 5 – Homogeneous CO2 Hydrogenation

5.1 Introduction

5.2 Homogeneous Carbon Dioxide Hydrogenation to Formic Acid and Formate

5.2.1 Ruthenium Catalysts

5.2.2 Rhodium Catalysts

5.2.3 Iridium Catalysts

5.2.4 Non-precious Metal Catalysts

5.3 Homogeneous Carbon Dioxide Hydrogenation to Methanol

5.3.1 Ruthenium Catalysts

5.3.2 Other Metal Catalysts

5.3.3 Metal-free Catalysts

5.4 Mechanistic Aspects

5.5 Conclusions

References

Chapter 6 – Homogeneous CO2 Copolymerization and Coupling

6.1 Introduction

6.2 Epoxide Copolymerization with CO2

6.3 Olefin Coupling with CO2

6.4 Conclusions and Outlook

References

Chapter 7 – Heterogeneous CO2 Hydrogenation

7.1 Introduction

7.2 CO2 to Methanol

7.3 CO2 to Dimethyl Ether (DME)

7.4 CO2 to Formic Acid and Formates

7.5 CO2 to Higher Alcohols

7.6 CO2 to Liquid Fuel

7.7 CO2 to Lower Olefins

7.8 CO2 to Aromatics

7.9 Conclusions

Acknowledgements

References

Chapter 8 – CO2 Methanation

8.1 Introduction

8.2 Thermodynamics

8.3 Catalysts

8.4 Mechanisms

8.4.1 Mechanism on Unsupported Catalysts

8.4.2 Mechanism on Supported Catalysts

8.5 Kinetics

8.6 Reactors

8.7 Conclusions

Acknowledgements

References

Chapter 9 – Methane Dry Reforming

9.1 Dry Reforming – Technology Comparison and Economical Potential

9.2 Mechanistic Considerations

9.3 Coking and Sintering as the Main Challenges for Catalyst Materials for Dry Reforming

9.4 Catalyst Design

9.4.1 Prevention of Sintering through Catalyst Design

9.4.1.1 Catalyst Support Materials as a Vital Element in the Prevention of Sintering – Engineering

9.4.1.2 Encapsulated Active Metals – Core Shell Approaches

9.4.1.3 Synthetic Methods to Control Active Metal Dispersion and Particle Size

9.4.1.4 Alloying of Active Metals

9.4.2 Prevention of Coke Formation Through Catalyst Design

9.4.2.1 Supported Platinum Group Metals

9.4.2.2 Redox Active Metals and Support Materials

9.4.2.3 Encapsulated Active Metals/Core–Shell Approaches

9.4.2.4 Methods to Control Active Metal Dispersion and Particle Size

9.5 Conclusions

List of Abbreviations

Acknowledgements

References

Chapter 10 – Gas-phase CO2 Recycling via the Reverse Water–Gas Shift Reaction: A Comprehensive Ove

10.1 Background

10.2 Potential Industrial Applications

10.3 Thermodynamic Analysis

10.4 Mechanism Considerations

10.4.1 The Redox Mechanism

10.4.2 The Associative Mechanism

10.5 Catalyst Design

10.5.1 Non-noble-metal-based Catalysts

10.5.1.1 Ni-based Catalysts

10.5.1.2 Cu-based Catalysts

10.5.1.3 Fe-based Catalysts

10.5.2 Hybrid-metal-oxide Catalysts

10.5.3 Carbide-support Catalysts

10.6 Summary and Outlook

Acknowledgements

References

Chapter 11 – Heterogeneous Copolymerization of CO2

11.1 Introduction

11.1.1 Initial Findings in Copolymerization of CO2 and an Epoxide

11.2 Development of the Zinc Glutarate Systems

11.2.1 Effect of Supports, Templates, and Additives in ZnGA Synthesis

11.2.2 Zinc Adipates and Zinc Pimelates

11.2.3 Terpolymerization Using Zn-dicarboxylate Catalysts

11.2.4 Solid-state Structure and Mechanistic Studies

11.3 Double Metal Cyanide Complexes as Heterogeneous Catalysts

11.4 Summary and Outlook

Acknowledgements

References

Chapter 12 – Artificial Photosynthesis for Production of Solar Fuels and Chemicals

12.1 Introduction

12.2 Natural Photosynthesis as the Blueprint for Artificial Photosynthetic Systems

12.2.1 Molecular Principles of Oxygenic Photosynthesis

12.3 Photoelectrochemical CO2 Reduction

12.3.1 General Principles

12.3.2 Products of Photoelectrochemical CO2 Reduction

12.3.2.1 Carbon Monoxide (CO)

12.3.2.1 Carbon Monoxide (CO)

12.3.2.2 Formate and Formic Acid

12.3.2.3 Methanol

12.3.2.4 Methane

12.3.2.5 Ethanol

12.3.3 Electrocatalytic Conversion Systems with Integrated PV Modules

12.4 Semi-artificial Photosynthetic Systems for Solar-driven CO2 Reduction

12.4.1 Biomolecular (Enzymatic) Solar-to-Fuel Systems

12.4.2 Biohybrid Systems with Microbial Cell Factories

12.5 Future Outlook

Acknowledgements

References

Chapter 13 – Photocatalytic CO2 Reduction Reactions

13.1 Introduction

13.2 Basic Considerations of Photocatalytic CO2 Reduction Reactions

13.2.1 Mechanisms of Photocatalytic CO2 Reduction

13.2.2 Challenges of Photocatalytic CO2 Reduction Reactions

13.2.3 Performance Evaluation of Photocatalytic CO2 Reduction

13.2.3.1 Activity

13.2.3.2 Product Selectivity

13.3 Influence Factors of Photocatalytic CO2 Reduction Performance

13.3.1 The Light-absorption Range and CB Position of Photocatalyst

13.3.2 The Transfer and Separation of Photogenerated Charge Carriers

13.3.3 Surface Catalytic Reaction Rate

13.3.4 Adsorption/Desorption of Reactants/Intermediates

13.3.5 Local Density of the Photogenerated Charge Carriers

13.4 Design Strategies of High-efficiency CO2 Reduction Photocatalyst

13.4.1 Tuning the Band Structure by Impurity Doping

13.4.2 Local Surface Plasmon Resonance (LSPR)

13.4.3 Strategies for Transfer and Separation of Photogenerated Charge Carriers

13.4.4 Surface Vacancies

13.4.5 Single-atom Active Sites

13.4.6 Surface Functional Group Modification

13.5 Conclusions and Perspectives

Acknowledgements

References

Chapter 14 – Plasmonic Photoreactors for Photocatalytic CO2 Conversion

14.1 CO2 Photocatalytic Conversion: From the Promise to the Reality

14.1.1 The Potential of Solar Energy

14.1.2 Thermodynamics: The Limits of Solar Energy Conversion

14.1.3 Concepts for the Integration of Solar Energy in Chemical Processes

14.1.4 Requirements for Industrial Scale Solar Fuels

14.1.5 Basic Elements of Photocatalytic Reactor Design

14.1.5.1 Radiation Model

14.1.5.2 Kinetic Model

14.1.6 The Reactor Boundaries

14.2 Plasmonic Microreactor: A Light Harvesting Device Concept

14.2.1 The Concept

14.2.2 Fabrication

14.2.3 Test

14.3 Plasmonic Materials

14.3.1 Main Materials Used

14.3.2 Main Synthesis Routes

14.3.3 Other Applications of the Plasmonic Materials

14.4 Conclusions and Outlook

Acknowledgements

References

Chapter 15 – Solar-thermal Catalytic CO2 Splitting

15.1 Solar Thermochemical Fuel Production

15.2 CeO2 for CO2 Splitting

15.3 Pure CeO2 for the Solar Thermochemical Splitting of CO2

15.4 Doping of CeO2 for Improved Thermochemical CO2 Production

15.4.1 Doping with Zirconia

15.4.2 Doping with Hafnium and Other Metals

15.5 Conclusions

References

Chapter 16 – Electrochemical CO2 Reduction

16.1 Introduction

16.2 Heterogeneous Catalysts for CO2 Reduction Reaction

16.2.1 Strategy for C1 Selectivity

16.2.1.1 Carbon Monoxide

16.2.1.2 Formic Acid or Formate

16.2.1.3 Formaldehyde

16.2.1.4 Methanol

16.2.1.5 Methane

16.2.2 Strategy for C2/Cn Selectivity

16.2.2.1 Ethylene

16.2.2.2 Ethanol

16.2.2.3 Cn Products

16.3 Homogeneous Catalysts

16.3.1 Introduction

16.3.2 Heterogenized Systems

16.3.3 Reduction of CO2 with Two Electrons

16.3.3.1 Mechanistic Insights

16.3.4 Reduction of CO2 Beyond Two Electrons

16.3.4.1 Formaldehyde

16.3.4.2 Methanol

16.3.4.3 Methane

16.3.5 Reduction of CO2 Coupled to C–C Bond Formation

16.3.5.1 Oxalate

16.3.5.2 Higher Reduction Products

16.4 Frontiers Between Homo-/Heterogeneous Catalysts

16.4.1 Single Atom Catalysts

16.5 Operando Characterization

16.5.1 Infrared Spectroscopy

16.5.2 Raman Spectroscopy

16.5.3 X-ray Absorption Spectroscopy (XAS)

16.5.4 X-ray Photoelectron Spectroscopy (XPS)

16.5.5 Necessity for Labelled Studies

16.5.6 DEMS as a New and Complementary Spectroscopic Method

16.6 Concluding Remarks

References

Chapter 17 – Advances in Electrochemical Carbon Dioxide Reduction Toward Multi-carbon Products

17.1 Introduction

17.2 Molecular Scale: Electrocatalysts, Mechanisms and Electrolyte Effects for CO2RR to Multi-carbon

17.2.1 Copper Based Electrocatalysts

17.2.2 Copper-based Multi-metallic Electrocatalysts

17.2.3 Non-copper Based Electrocatalysts for the Production of Multi-carbon Products

17.2.4 Cascade Electrocatalysis

17.2.5 Electrolyte Effects

17.3 Electrolyser Scale: Cell Designs and Components

17.3.1 Electrochemical H-cells

17.3.2 Gas Diffusion Electrodes

17.3.3 Three-chamber GDE Flow Cells

17.3.4 Membrane Electrode Assembly Cells

17.3.5 Electrolyser Stacks

17.3.6 Promising Results at the Electrolyser Scale

17.4 Process Scale: Integrating the CO2RR to Multi-carbon Products into a Process

17.4.1 Product Selection

17.4.2 Electricity Costs

17.4.3 Product Separation

17.4.4 Integrated Process Design

17.5 Conclusion

Acknowledgements

References

Chapter 18 – Techno-economic Analysis of CO2 Electroreduction

18.1 CO2 Electroreduction Framework

18.2 Modelling and Assessment Methodology

18.2.1 System Boundaries and Carbon Footprint Evaluation

18.2.2 Metrics and Proposed Methods in the Economic Evaluation

18.3 Analysis of Trends in CO2 Conversion by Electrochemical Reduction

18.3.1 Case Study of Formic Acid: Techno-economic Figures for Electrochemical Production

18.3.2Environmental Feasibility of CO2-based Products

18.3.3 Profitability of the CO2 Electroreduction Products

18.4 Remaining Challenges

Appendix

References

Chapter 19 – Microwave-assisted Catalytic Dry Methane Reforming

19.1 Introduction

19.2 Interaction of Microwaves with Solid Catalysts

19.3 Catalyst Development for Microwave-assisted Dry Methane Reforming

19.4 Reactor Design and Scale-up Aspects of Microwave-assisted Dry Methane Reforming

19.5 Alternative Electricity-based Heating Techniques for (Dry) Methane Reforming

19.6 Conclusions

References

Chapter 20 – CO2 Hydrogenation With a Dielectric Barrier Discharge Reactor

20.1 Introduction

20.2 Hydrogenation of CO2 with DBD Reactors

20.2.1 DBD Plasma Reactors

20.2.2 Plasma Hydrogenation of CO2

20.2.3 Gas Phase Reaction Mechanism of Plasma CO2 Hydrogenation

20.3 Plasma-catalytic Hydrogenation of CO2 in a Packed-bed DBD Reactor

20.3.1 Combination of Plasma with Catalysts

20.3.2 Catalyst Material

20.3.3 Mechanism of Plasma-catalytic CO2 Hydrogenation

20.4 Conclusion and Outlook

Acknowledgements

References

Chapter 21 – CO2 Splitting With Nanosecond Pulsed Discharge

21.1 Introduction

21.2 CO2 Dissociation Reactions

21.3 Non-thermal Plasma (NTP) Technologies for CO2 Splitting

21.3.1 Dielectric Barrier Discharge (DBD)

21.3.2 Corona and Spark Discharges

21.3.3 Microwave (MW) and Radio-frequency (RF) Discharges

21.3.4 Gliding Arc Discharge (GAD)

21.3.5 Nanosecond Pulsed Discharge (NPD)

21.4 CO2 Splitting in NPD Driven Reactors: A Thorough Parametric Study

21.4.1 Impact of Specific Energy Input (SEI)

21.4.2 Impact of Pressure

21.4.3 Impact of Interelectrode Gap

21.4.4 Impact of Promoter Gas Addition

21.4.5 Impact of Packing Material

21.5 Plasma Diagnostics

21.6 Plasma Modelling

21.7 Conclusions

References

Chapter 22 – Valorisation of Carbon Dioxide via Enzymatic Transformation

22.1 Introduction

22.2 CO2 Converting Enzymes

22.2.1 Carbonic Anhydrase versus Formate Dehydrogenase Catalysis

22.3 Enzymatic Cascade Conversion of CO2 to Chemicals

22.4 FDH Enzymes

22.4.1 Metal Dependent FDHs: Recent Progress

22.5 Significance of the Electron Donors Supporting FDH Catalysed CO2 Reduction

22.6 Enzyme Robustness

22.7 Conclusions and Perspectives

Acknowledgements

References

Chapter 23 – Microbial CO2 Conversion Routes

23.1 Introduction

23.2 Major Advantages and Challenges

23.3 Main CO2 Fixating Microbes and Related Pathways

23.4 Most Promising Products and Process Configurations

23.5 Strategies to Improve CO2 Conversion Efficiency

23.6 Outlook, Future Prospects and Conclusions

23.6.1 Outlook and Future Prospects

23.6.2 Conclusions

List of Abbreviations

Acknowledgements

References

Chapter 24 – Hydrothermal CO2 Reduction Using Metals and Biomass Derivatives as Reductants

24.1 Hydrothermal CO2 Reduction Processes in Nature

24.2 Hydrothermal CO2 Reduction with Metals as Reductants: an Overview

24.3 Mechanisms and Kinetics of Hydrothermal CO2 Reduction with Metals

24.4 Comparison of Different Carbon Sources

24.5 Hydrothermal Decomposition and Fractionation of Lignocellulosic Biomass Waste

24.6 Screening of Organic Reductants Obtained by Hydrothermal Fractionation of Biomass

24.7 Mechanisms of the Hydrothermal Reduction with Organic Derivatives of Biomass

24.8 A Continuous Flow Reactor for the Hydrothermal Reduction of CO2 with Organic Biomass Derivative

24.9 Conclusions

Acknowledgements

References

Chapter 25 – Life Cycle Analysis of CO2 Valorisation

25.1 Introduction

25.2 Life Cycle Assessment

25.2.1 Definition of the Goal and Scope

25.2.2 Life Cycle Inventory Analysis

25.2.3 Life Cycle Impact Assessment

25.2.4 Interpretation

25.3 Environmental Impacts of CO2 Valorisation

25.3.1 Methane

25.3.2 Methanol

25.3.3 CO

25.3.4 DME

25.3.5 DMC

25.3.6 Polyols

25.3.7 Normalised Results

25.4 Conclusion and Recommendations

Acknowledgements

References

Subject Index

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