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Table of contents
Introduction
Goals of doctoral thesis
Abbreviations
Chapter 1 – Current status and literature review on CO2 utilization
1.1. CO2 and climate
1.2. Reduction of CO2 emissions – solutions and technologies
1.2.1. Carbon dioxide capture and storage (CCS)
1.2.2. Current and emerging carbon dioxide utilization technologies
1.2.2.1. Chemicals production – mature technologies
1.2.2.2. Chemicals production – mature and emerging technologies, and future prospects
1.3. Tri-reforming of methane: reactions, mechanism and catalysts
1.3.1. Two concepts of tri-reforming of methane
1.3.1.1. Flue gases from natural gas power station for tri-reforming of methane
1.3.1.2. CO2 separation for tri-reforming of methane
1.3.2. Tri-reforming of methane (TRM): three main reactions
1.3.2.1. Dry reforming of methane (DRM)
1.3.2.2. Steam reforming of methane (SRM)
1.3.2.3. Partial oxidation of methane (POM)
1.3.2.4. Autothermal steam reforming (ATR)
1.3.2.5. Combined dry reforming and partial oxidation of methane (CRPOM)
1.3.3. Catalysts for tri-reforming of methane
1.3.3.1. Dry reforming of methane (DRM)
1.3.3.2. Steam reforming of methane (SRM)
1.3.3.3. Partial oxidation of methane (POM)
1.3.4. Double layered-hydroxides as potential catalysts for tri-reforming of methane
1.3.4.1. Properties, synthesis and application
1.3.4.2. Double layered-hydroxides in methane reforming processes
Chapter 2 – Experimental part
2.1. Catalyst preparation
2.1.1. Co-precipitation technique
2.1.2. Co-impregnation technique
2.1.3. Incipient wetness impregnation
2.2. Characterization methods
2.2.1. X-ray diffraction (XRD)
2.2.2. X-ray fluorescence (XRF)
2.2.3. Low temperature nitrogen sorption
2.2.4. Temperature programmed reduction (TPR-H2)
2.2.5. Temperature programmed desorption (TPD-CO2)
2.2.6. H2 chemisorption
2.2.7. Transmission Electron Microscopy (TEM)
2.2.8. High-Resolution Electron Microscopy (HRTEM)
2.2.9. Thermogravimetric analysis coupled by mass spectroscopy (TGA/MS)
2.2.10. Raman spectroscopy
2.3. Catalytic tests
2.4. Thermodynamic calculations
2.4.1 Minimization of Gibbs free energy
2.4.2. Calculation method
Chapter 3 – Thermodynamic analysis of DRM, SRM, POM, TRM
3.1. Thermodynamic equilibrium analysis of methane reforming processes
3.1.1. Dry reforming of methane calculations
3.1.2. Dry reforming of methane versus other reforming processes
3.1.3. The influence of feed gas composition on carbon deposition
3.2. Thermodynamic calculations for tri-reforming of methane assuming direct application of CO2 from flue gases
3.3. Conclusions
Chapter 4 – Dry reforming of methane (DRM)
4.1. Yttrium promotion of Ni-based double layered-hydroxides
4.1.1. Physicochemical properties
4.1.2. Reducibility, basicity, Ni dispersion and crystallite size
4.1.3. Catalytic activity and stability in DRM
4.1.4. Characterization of the spent catalysts
4.1.5. Conclusions
4.2. Co-impregnation with zirconium and yttrium of Ni-based double layered-hydroxides
4.2.1. Physicochemical properties
4.2.2. Reducibility, basicity, Ni dispersion and crystallite size
4.2.3. Catalytic activity and stability in DRM
4.2.4. Characterization of the spent catalysts after the TPSR test
4.2.5. Characterization of the spent catalysts after the isothermal tests
4.2.6. Conclusions
4.3. Co-precipitation with zirconium and impregnation with yttrium versus co-precipitation with zirconium and yttrium
4.3.1. Physicochemical properties
4.3.2. Reducibility, basicity, Ni dispersion and crystallite size
4.3.3. Catalytic activity and stability in DRM
4.3.4. Characterization of the spent catalysts after the isothermal tests
4.3.5. Conclusions
4.4. Co-precipitation with cerium and impregnation with yttrium of Ni-based double layeredhydroxides
4.4.1. Physicochemical properties
4.4.2. Reducibility, basicity, Ni dispersion and crystallite size
4.4.3. Catalytic activity and stability in DRM
4.4.4. Characterization of the spent catalysts after the isothermal tests
4.4.5. Conclusions
4.5. Overall conclusions on dry reforming of methane
Chapter 5 – Tri-reforming of methane and other reactions on selected catalysts
5.1. Partial oxidation of methane – one of main reactions in tri-reforming of methane
5.1.1. TPSR catalytic tests
5.1.2. Isothermal catalytic tests of partial oxidation of methane
5.2. Combined CO2 reforming and partial oxidation of methane as a part of the process of trireforming of methane
5.3. Tri-reforming of methane
5.3.1. Feed gas composition of (CH4/CO2/H2O/O2/Ar=1/0.5/0.5/0.1/7.9)
5.3.1.1. Catalytic tests
5.3.1.2. Characterization of the spent catalysts
5.3.2. Gas composition of flue gases from natural-gas-fired power station (CH4/CO2/H2O/O2/Ar = 3/1/2/0.3/3.7)
5.3.2.1. Catalytic tests
5.3.2.2. Characterization of the spent catalysts
5.4. The comparison of HTNi and HTNi-Y2.0 catalysts in DRM, POM, CRPOM and TRM
5.5. Conclusions
General conclusions
References
