CO2 Methanation: Nickel–Alumina Catalyst Prepared by Solid-State Combustion
Abstract
:1. Introduction
2. Materials and Methods
2.1. Synthesis of Hexakis-(Imidazole) Nickel (II) Nitrate Complex
2.2. Catalyst Preparation
2.3. Catalyst Characterization
2.4. Experimental Setup
3. Results and Discussion
3.1. Study of the Organometallic Precursor of the Nickel–Alumina Catalyst
3.2. Study of Nickel–Alumina Catalyst
3.2.1. Catalyst Composition
3.2.2. Local Analysis of Catalyst Particles
3.2.3. State of Nickel on the Catalyst Surface
3.2.4. Porous Structure of Catalysts
3.3. Study of CO2 Methanation
3.3.1. Catalyst Activation
3.3.2. Catalyst Activity in CO2 Methanation
4. Conclusions
Supplementary Materials
Author Contributions
Funding
Institutional Review Board Statement
Informed Consent Statement
Data Availability Statement
Acknowledgments
Conflicts of Interest
References
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Catalyst | Metal Content, wt% | In Terms of Weight Per cent Oxides, wt% | Molar Ratio Ni/Al | ||
---|---|---|---|---|---|
Al | Ni | Al2O3 | NiO | ||
Ni-Al2O3-SSC | |||||
calculated | 42.4 | 15.7 | 80 | 20 | 0.17 |
found | 29.8 | 16.4 | 56.4 | 20.8 | 0.25 |
NIAP-07-01 | |||||
found | 23.4 | 24.7 | 44.1 | 31.3 | 0.48 |
Sample | Phase | Lattice Parameter of γ-Al2O3, Å | PDF Card |
---|---|---|---|
initial Al2O3 | γ-Al2O3 | 7.918 | 10-425 |
Ni-Al2O3-SSC | γ-Al2O3 | 7.921 | 10-425 |
NiO | 47-1049 | ||
NIAP-07-01 | γ-Al2O3 | 7.931 | 10-425 |
NiO | 47-1049 | ||
Graphite | 41-1487 |
Catalyst | Surface Area, m2·g−1 | Pore Volume, m3·g−1 | Average Pore Diameter, nm |
---|---|---|---|
Ni-Al2O3-SSC | 157 | 0.35 | 8.8 |
NIAP-07-01 | 150 | 0.35 | 9.2 |
Catalyst Preparation Method | Thermal Treatment Conditions | Reduction Conditions | Reaction Conditions | Ni Content, wt% | Temperature, °C | CO2 Conversion *, % | Reference |
---|---|---|---|---|---|---|---|
SSC | - | H2:CO2:Ar = 16:4:80; 100 mL·min−1;350 °C; 20 min | GHSV—19,000 mL·gcat−1·h−1 H2:CO2:Ar = 16:4:80 H2/CO2 = 4 | 16.4 | 150 | 2 | This work |
200 | 3 | ||||||
250 | 17 | ||||||
300 | 54 | ||||||
350 | 69 | ||||||
NIAP-07-01 | 24.7 | 150 | 0 | ||||
200 | 0 | ||||||
250 | 2 | ||||||
300 | 9 | ||||||
350 | 26 | ||||||
Ultrasound assisted co-precipitated | 700 °C, 4 h | Pure H2; 25 mL·min−1; 600 °C; 2 h | GHSV—9000 mL·gcat−1·h−1 H2:CO2 = 3.5 | 15 | 250 | 0 | [43] |
300 | 2 | ||||||
350 | 18 | ||||||
20 | 200 | 0 | |||||
250 | 6 | ||||||
300 | 58 | ||||||
350 | 70 | ||||||
Wet impregnation | 700 °C, 5 h | 20%H2 in helium; 700 °C; 1 h | GHSV—52,300 h−1H2:CO2 = 5 without any dilution; mcat = 44 mg | 16 | 250 | 1 | [62] |
300 | 6 | ||||||
400 | 50 | ||||||
500 | 75 | ||||||
39 | 250 | 2 | |||||
300 | 8 | ||||||
400 | 78 | ||||||
500 | 81 | ||||||
Wet impregnation in presence of citric acid | 400 °C, 2 h | Pure H2; 80 mL·min−1; 600 °C; 2 h | GHSV—30,000 mL·gcat−1·h−1 H2:CO2:Ar = 61.6:15.4:23 H2:CO2 = 3.99 | 10 | 200 | 2 | [17] |
240 | 8 | ||||||
280 | 39 | ||||||
320 | 81 | ||||||
20 | 200 | 3 | |||||
240 | 19 | ||||||
280 | 67 | ||||||
320 | 90 | ||||||
Wetness incipient impregnation | 500 °C, 4 h | 20% H2 in helium 300 mL·min−1 500 °C 1 h | GHSV—10,000 h−1 H2:CO2:He = 5:1:1.5 H2:CO2—5 | 16 | 200 | 1 | [37] |
250 | 5 | ||||||
300 | 21 | ||||||
350 | 65 | ||||||
20 | 200 | 1 | |||||
250 | 7 | ||||||
300 | 32 | ||||||
350 | 71 | ||||||
Wet impregnation | 450 °C, 2 h | Pure H2; 25 mL·min−1; 450 °C; 2 h | GHSV—9000 mL·gcat−1·h−1 H2:CO2 = 3.5 | 15 | 200 | 4 | [64] |
250 | 10 | ||||||
300 | 47 | ||||||
350 | 70 | ||||||
20 | 200 | 8 | |||||
250 | 42 | ||||||
300 | 74 | ||||||
350 | 78 | ||||||
Wetness incipient impregnation | 800 °C, 2 h | Pure H2 stream; 500 °C; 2 h | GHSV—60,000 mL·gcat−1·h−1 H2:CO2 = 4 | 15 | 250 | 1 | [29] |
300 | 52 | ||||||
350 | 77 | ||||||
Solution combustion synthesis | 400 °C, 4 h | Pure H2 30 mL·min−1; 400 °C; 2 h | GHSV—3600 mL·gcat−1·h−1 H2:CO2 = 4 | 20 | 250 | 44 | [34] |
300 | 84 | ||||||
350 | 85 | ||||||
Solution combustion synthesis | 600 °C, 2 h | 50% H2 in N2; 40 mL·min−1; 600 °C; 1 h | GHSV—10,000 h−1 H2:CO2:CO:N2 = 39:6.1:4.9:50 | 15 | 300 | 0 | [45] |
350 | 29 | ||||||
Sulfactant-free sol-gel | 700 °C, 3 h | Pure H2 25 mL·min−1; 600 °C; 2 h | GHSV—9000 mL·gcat−1·h−1 H2:CO2 = 3.5 without any dilution | 15 | 200 | 1 | [40] |
250 | 14 | ||||||
300 | 61 | ||||||
350 | 72 | ||||||
20 | 200 | 2 | |||||
250 | 17 | ||||||
300 | 65 | ||||||
350 | 72 | ||||||
Wetness incipient impregnation | 600 °C, 4 h | Pure H2 60 mL·min−1; 600 °C; 1 h | GHSV—16,000 h−1 H2:CO2 = 4 in N2 | 15 | 200 | 3 | [65] |
250 | 10 | ||||||
300 | 28 | ||||||
350 | 48 |
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Netskina, O.; Mucha, S.; Veselovskaya, J.; Bolotov, V.; Komova, O.; Ishchenko, A.; Bulavchenko, O.; Prosvirin, I.; Pochtar, A.; Rogov, V. CO2 Methanation: Nickel–Alumina Catalyst Prepared by Solid-State Combustion. Materials 2021, 14, 6789. https://doi.org/10.3390/ma14226789
Netskina O, Mucha S, Veselovskaya J, Bolotov V, Komova O, Ishchenko A, Bulavchenko O, Prosvirin I, Pochtar A, Rogov V. CO2 Methanation: Nickel–Alumina Catalyst Prepared by Solid-State Combustion. Materials. 2021; 14(22):6789. https://doi.org/10.3390/ma14226789
Chicago/Turabian StyleNetskina, Olga, Svetlana Mucha, Janna Veselovskaya, Vasily Bolotov, Oxana Komova, Arkady Ishchenko, Olga Bulavchenko, Igor Prosvirin, Alena Pochtar, and Vladimir Rogov. 2021. "CO2 Methanation: Nickel–Alumina Catalyst Prepared by Solid-State Combustion" Materials 14, no. 22: 6789. https://doi.org/10.3390/ma14226789