Influence of Synthesis Conditions on Catalytic Performance of Ni/CeO2 in Aqueous-Phase Hydrogenolysis of Glycerol without External Hydrogen Input
Abstract
:1. Introduction
2. Results and Discussion
2.1. Catalyst Characterization Results before the Reaction
2.1.1. Chemical Analysis and Textural Properties
2.1.2. X-ray Diffraction
2.1.3. H2-TPR Results
2.1.4. NH3-TPD Results
2.2. Catalytic Activity
2.2.1. Global Activity Results
2.2.2. Products Distribution
2.3. Catalyst Characterization Results after the Reaction
2.3.1. X-ray Diffraction
2.3.2. SEM Microscopy
2.3.3. Elemental Analysis
3. Materials and Methods
3.1. Catalyst Preparation
3.2. Catalyst Characterization
3.3. Catalyst Performance
4. Conclusions
Supplementary Materials
Author Contributions
Funding
Data Availability Statement
Acknowledgments
Conflicts of Interest
References
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Ni Content (wt.%) | Surface Area (m2/g) | Pore Volume (cm3/g) | Pore Diameter (nm) | Metallic Dispersion, Dexp (%) | |
---|---|---|---|---|---|
Ni10/CeO2(500)600 | 9.644 ± 0.085 | 67 | 0.15 | 8.8 | 1.90 |
Ni10/CeO2(500)700 | 9.793 ± 0.098 | 54 | 0.14 | 10.0 | 2.72 |
Ni10/CeO2(500)800 | 9.418 ± 0.066 | 22 | 0.07 | 12.7 | 1.13 |
Ni10/CeO2(700)700 | 9.592 ± 0.013 | 34 | 0.11 | 12.9 | 1.85 |
Ni20/CeO2(500)700 | 19.670 ± 0.089 | 38 | 0.13 | 13.4 | 1.62 |
CeO2(500) | - | 98 | 0.23 | 9.4 | - |
CeO2(700) | - | 61 | 0.19 | 11.5 | - |
Temperatures (°C) | |||||
---|---|---|---|---|---|
T1 | T2 | T3 | T4 | T5 | |
Ni10/CeO2(500)600 | 172 | 218 | 309 | 335 | 798 |
Ni10/CeO2(500)700 | 182 | 224 | 320 | 367 | 807 |
Ni10/CeO2(500)800 | 196 | 204 | 308 | 491 | 810 |
Ni10/CeO2(700)700 | 160 | 213 | 309 | 413 | 812 |
Ni20/CeO2(500)700 | 171 | 227 | 341 | 444 | 823 |
Temperatures (°C) | Strength of Acid Sites * (%) | TASmass | TASsurface | |||||||
---|---|---|---|---|---|---|---|---|---|---|
T1 | T2 | T3 | T4 | L | L-M | M | H | µmol NH3/g | µmol NH3/m2 | |
CeO2(500) | 245 | 413 | 528 | 675 | - | 16 | 50 | 34 | 64 | 0.65 |
CeO2(700) | 241 | 372 | 551 | 740 | - | 20 | 57 | 23 | 18 | 0.30 |
Ni10/CeO2(500)600 | 163 | 223 | 346 | - | 24 | 67 | 8 | - | 196 | 2.93 |
Ni10/CeO2(500)700 | 151 | 238 | 362 | - | 32 | 53 | 15 | - | 151 | 2.80 |
Ni10/CeO2(500)800 | 145 | 219 | 337 | - | 27 | 68 | 5 | - | 58 | 2.64 |
Ni10/CeO2(700)700 | 145 | 227 | 367 | - | 28 | 56 | 16 | - | 78 | 2.29 |
Ni20/CeO2(500)700 | 146 | 231 | 361 | - | 34 | 49 | 17 | - | 144 | 3.79 |
Ni10/CeO2(500)600 | Ni10/CeO2(500)700 | Ni10/CeO2(500)800 | Ni10/CeO2(700)700 | Ni20/CeO2(500)700 | |
---|---|---|---|---|---|
Global catalyst performance | |||||
Gly. conv. (%) | 19.1 ± 0.9 | 29.0 ± 0.3 | 17.1 ± 0.1 | 25.5 ± 0.1 | 23.5 ± 0.9 |
CYliq (%) | 15.7 ± 0.8 | 21.4 ± 0.5 | 12.6 ± 0.5 | 24.0 ± 0.1 | 18.2 ± 0.3 |
CYgas (%) | 1.4 ± 0.2 | 1.1 ± 0.1 | 0.8 ± 0.5 | 1.5 ± 0.9 | 1.9 ± 0.1 |
Cdef (%) | 2.0 | 6.5 | 3.7 | 0 | 3.4 |
TONsurface (molgly·m2/molH+) | 95 | 190 | 98 | 145 | 96 |
TONmass (molgly·g/molH+) | 79 | 175 | 249 | 251 | 139 |
Selectivity (%) | |||||
1,2-PDO | 40 ± 1 | 33 ± 1 | 31 ± 1 | 23 ± 2 | 41 ± 1 |
Acetol | 39 ± 1 | 44 ± 2 | 51 ± 1 | 59 ± 3 | 33 ± 1 |
Acetone | 0.54 ± 0.05 | 0.54 ± 0.01 | 0.48 ± 0.01 | 0.82 ± 0.01 | 0.47 ± 0.03 |
EG | 7.6 ± 0.1 | 6.3 ± 0.4 | 6.0 ± 0.1 | 4.5 ± 0.5 | 8.4 ± 0.2 |
EtOH | 11.8 ± 0.3 | 12.4 ± 0.7 | 9.3 ± 0.1 | 11.6 ± 0.5 | 13.8 ± 0.7 |
Acetic acid | 0.9 ± 0.1 | 3.1 ± 0.1 | 1.2 ± 0.2 | - | 2.8 ± 0.3 |
MeOH | 0.9 ± 0.1 | 0.7 ± 0.1 | 0.8 ± 0.2 | 1.2 ± 0.3 | 0.8 ± 0.1 |
Yields (gA/gglycerol) | |||||
1,2-PDO | 0.0513 | 0.058 | 0.0327 | 0.0458 | 0.0613 |
Acetol | 0.0486 | 0.0758 | 0.0514 | 0.1136 | 0.0484 |
EG | 0.012 | 0.0136 | 0.0076 | 0.0109 | 0.0154 |
EtOH | 0.0138 | 0.0198 | 0.0088 | 0.0209 | 0.0188 |
Carbon (wt.%) | Ni (wt.%) | Ce (wt.%) | |
---|---|---|---|
Ni10/CeO2(500)600 | 3.83 | 0.39 | 0.35 |
Ni10/CeO2(500)700 | 3.88 | 0.30 | 0.08 |
Ni10/CeO2(500)800 | 2.38 | 0.25 | 0.07 |
Ni10/CeO2(700)700 | 1.88 | 0.35 | 0.40 |
Ni20/CeO2(500)700 | 3.96 | 0.13 | 0.04 |
Catalyst | T1 (°C) | T2 (°C) | Nickel Load (wt.%) | Reduction Temp. (°C) |
---|---|---|---|---|
Ni10/CeO2(500)600 | 500 | 600 | 10 | 500 |
Ni10/CeO2(500)700 | 500 | 700 | 10 | 500 |
Ni10/CeO2(500)800 | 500 | 800 | 10 | 550 |
Ni10/CeO2(700)700 | 700 | 700 | 10 | 500 |
Ni20/CeO2(500)700 | 500 | 700 | 20 | 500 |
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Jarauta-Córdoba, C.; García, L.; Ruiz, J.; Oliva, M.; Arauzo, J. Influence of Synthesis Conditions on Catalytic Performance of Ni/CeO2 in Aqueous-Phase Hydrogenolysis of Glycerol without External Hydrogen Input. Molecules 2024, 29, 3797. https://doi.org/10.3390/molecules29163797
Jarauta-Córdoba C, García L, Ruiz J, Oliva M, Arauzo J. Influence of Synthesis Conditions on Catalytic Performance of Ni/CeO2 in Aqueous-Phase Hydrogenolysis of Glycerol without External Hydrogen Input. Molecules. 2024; 29(16):3797. https://doi.org/10.3390/molecules29163797
Chicago/Turabian StyleJarauta-Córdoba, Clara, Lucía García, Joaquín Ruiz, Miriam Oliva, and Jesús Arauzo. 2024. "Influence of Synthesis Conditions on Catalytic Performance of Ni/CeO2 in Aqueous-Phase Hydrogenolysis of Glycerol without External Hydrogen Input" Molecules 29, no. 16: 3797. https://doi.org/10.3390/molecules29163797