Optimization of the Load of Transition Metal Oxides (Fe2O3, Co3O4, NiO and/or PdO) onto CeO2 Nanoparticles in Catalytic Steam Decomposition of n-C7 Asphaltenes at Low Temperatures
Abstract
:1. Introduction
2. Materials and Methods
2.1. Materials
2.2. Methods
2.2.1. Functionalization of CeO2 Nanoparticles with NiO, Fe2O3, Co3O4, and PdO
2.2.2. Characterization of the Nanoparticles
2.2.3. Equilibrium Adsorption Isotherms
2.2.4. Thermogravimetric Analysis of Asphaltenes
3. Modeling
3.1. Simplex-Centroid Mixture Design
3.2. Solid-Liquid Equilibrium (SLE) Model
3.3. Estimation of Activation Energy and Reaction Kinetic Rate
4. Results and Discussion
4.1. Nanoparticle Characterization
4.2. Asphaltene Adsorption onto Nanoparticles
4.3. Catalytic Steam Gasification of n-C7 Asphaltenes
4.3.1. Mass Loss Analysis
4.3.2. Analysis of the Gaseous Products Evolved during the Steam Gasification Process
4.3.3. Coke Yield
4.4. Effect of n-C7 Asphaltene Amount Adsorbed on the Decomposition Temperature
4.5. Maximization of Conversion of Asphaltenes during Steam Gasification through an SCMD
4.5.1. Isothermal Conversion of Asphaltenes Adsorbed on Nanoparticles from SCMD
4.5.2. Effective Activation Energy and Kinetics of the Catalytic Steam Gasification of Asphaltenes in the Presence and Absence of Nanoparticles
5. Conclusions
Supplementary Materials
Author Contributions
Funding
Acknowledgments
Conflicts of Interest
References
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Sample | Nominal Oxides | Nominal Mass Fraction (%) | Nominal Molar Fraction (%) |
---|---|---|---|
CeO2 | CeO2 | 100.0 | 100.0 |
CeNi1Pd1 | CeO2 | 98.0 | 98.8 |
NiO | 1.0 | 0.4 | |
PdO | 1.0 | 0.7 | |
CeFe1Pd1 | CeO2 | 98.0 | 98.4 |
Fe2O3 | 1.0 | 0.9 | |
PdO | 1.0 | 0.7 | |
CeCo1Pd1 | CeO2 | 98.0 | 97.9 |
Co3O4 | 1.0 | 1.4 | |
PdO | 1.0 | 0.7 | |
CeNi2 | CeO2 | 98.0 | 99.1 |
NiO | 2.0 | 0.9 | |
CePd2 | CeO2 | 98.0 | 98.6 |
PdO | 2.0 | 1.4 | |
CeNi1 | CeO2 | 99.0 | 99.6 |
NiO | 1.0 | 0.4 | |
CePd1 | CeO2 | 99.0 | 99.3 |
PdO | 1.0 | 0.7 | |
CeNi0.66Pd0.66 | CeO2 | 98.7 | 99.2 |
NiO | 0.7 | 0.3 | |
PdO | 0.7 | 0.5 |
Sample | SBET ± 0.1 m2·g−1 | dp (nm ± 0.2 nm) | Dispersion (%) | ||||
---|---|---|---|---|---|---|---|
NiO | Co3O4 | Fe2O3 | PdO | Ni/Co/Fe | Pd | ||
CeO2 | 67.0 | - | - | - | - | - | - |
CeNi1Pd1 | 63.8 | 6.4 | - | - | 3.9 | 12.7 | 38.6 |
CeFe1Pd1 | 64.1 | - | - | 5.4 | 6.9 | 11.2 | 12.8 |
CeCo1Pd1 | 64.4 | - | 1.9 | - | 6.1 | 18.1 | 20.4 |
Material | H ± 0.02 (mg·g−1) × 10−2 | K ± 0.08 (g·g−1) | qm ± 0.01 (g·g−1) | RSM (%) |
---|---|---|---|---|
CeO2 | 10.12 | 0.21 | 0.13 | 0.02 |
CePd1 | 7.19 | 0.29 | 0.16 | 0.03 |
CeNi1 | 7.34 | 0.03 | 0.15 | 0.04 |
CePd2 | 6.25 | 0.39 | 0.18 | 0.01 |
CeNi2 | 6.70 | 0.04 | 0.16 | 0.01 |
CeNi0.66Pd0.66 | 6.61 | 0.05 | 0.16 | 0.02 |
CeNi1Pd1 | 6.02 | 0.06 | 0.22 | 0.01 |
CeFe1Pd1 | 6.58 | 0.04 | 0.17 | 0.02 |
CeCo1Pd | 5.34 | 0.06 | 0.19 | 0.01 |
Ce Ni0.89Pd1.1 | 2.84 | 0.04 | 0.25 | 0.01 |
Sample | Temperature °C | (kJ) | Kinetic Rate (min−1) at 50% Conversion |
---|---|---|---|
n-C7 asphaltenes (without nanoparticles) | 360 | 211.5 | 0.012 |
370 | 0.018 | ||
380 | 0.032 | ||
CeO2 | 230 | 44.0 | 0.013 |
240 | 0.021 | ||
250 | 0.879 | ||
CeNi1Pd1 | 230 | 29.6 | 0.0187 |
240 | 0.0401 | ||
250 | 0.1002 | ||
CeNi0.89Pd1.1 | 230 | 0.029 | |
240 | 25.6 | 0.084 | |
250 | 0.179 |
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Medina, O.E.; Gallego, J.; Arias-Madrid, D.; Cortés, F.B.; Franco, C.A. Optimization of the Load of Transition Metal Oxides (Fe2O3, Co3O4, NiO and/or PdO) onto CeO2 Nanoparticles in Catalytic Steam Decomposition of n-C7 Asphaltenes at Low Temperatures. Nanomaterials 2019, 9, 401. https://doi.org/10.3390/nano9030401
Medina OE, Gallego J, Arias-Madrid D, Cortés FB, Franco CA. Optimization of the Load of Transition Metal Oxides (Fe2O3, Co3O4, NiO and/or PdO) onto CeO2 Nanoparticles in Catalytic Steam Decomposition of n-C7 Asphaltenes at Low Temperatures. Nanomaterials. 2019; 9(3):401. https://doi.org/10.3390/nano9030401
Chicago/Turabian StyleMedina, Oscar E., Jaime Gallego, Daniela Arias-Madrid, Farid B. Cortés, and Camilo A. Franco. 2019. "Optimization of the Load of Transition Metal Oxides (Fe2O3, Co3O4, NiO and/or PdO) onto CeO2 Nanoparticles in Catalytic Steam Decomposition of n-C7 Asphaltenes at Low Temperatures" Nanomaterials 9, no. 3: 401. https://doi.org/10.3390/nano9030401