CO2 Hydrogenation to Renewable Methane on Ni/Ru Modified ZSM-5 Zeolites: The Role of the Preparation Procedure
Abstract
:1. Introduction
2. Results and Discussion
2.1. Physico-Chemical Properties
2.2. Catalytic Activity for CO2 Hydrogenation to Methane
3. Experimental
3.1. Materials
3.2. Preparation of Seed Crystals
3.3. Synthesis of ZSM-5 Zeolite
3.4. Modification with Ni or/and Ru Nanoparticles of ZSM-5 Zeolite
3.5. Characterization
3.6. Catalytic Activity Measurements
4. Conclusions
Author Contributions
Funding
Data Availability Statement
Conflicts of Interest
References
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Sample | Phase Composition | Cell Parameters, Å | Crystallite Size, nm |
---|---|---|---|
10NiZSM-5 | NiO (Fm-3m) | 4.1815 (7) | 16 |
Spent 10NiZSM-5 | Ni (Fm-3m) | 3.5241 (4) | 33 |
5NiZSM-5 | NiO (Fm-3m) | 4.184 (2) | 13 |
Spent 5NiZSM-5 | Ni (Fm-3m) | 3.534 (1) | 15 |
5RuZSM-5 | RuO2 (P42/mnm) | 4.511 (1) 3.114 (1) | 19 |
Spent 5RuZSM-5 | Ru (P63/mmc) | 2.7098 (8) 4.285 (2) | 19 |
5Ni5RuZSM-5 | NiO (Fm-3m) RuO2 (P42/mnm) | 4.186 (3) 4.511 (1) 3.112 (1) | 9 21 |
Spent 5Ni5RuZSM-5 | Ni (Fm-3m) Ru (P63/mmc) | 3.533 (2) 2.699 (2) 4.271 (6) | 14 9 |
10Ni5RuZSM-5 | NiO (Fm-3m) RuO2 (P42/mnm) | 4.186 (1) 4.514 (1) 3.110 (1) | 10 21 |
Spent 10Ni5RuZSM-5 | Ni (Fm-3m) Ru (P63/mmc) | 3.5318 (9) 2.696 (4) 4.26 (1) | 19 7 |
Samples | SSA 1 (m2/g) | PV 2 (cm3/g) | Micropore Vol. 3 (cm3/g) | Micropore Surf. Area 3 (m2/g) |
---|---|---|---|---|
ZSM-5 | 307 | 0.177 | 0.095 | 231 |
5NiZSM-5 | 315 | 0.200 | 0.105 | 256 |
10NiZSM-5 | 322 | 0.189 | 0.107 | 261 |
5RuZSM-5 | 337 | 0.189 | 0.116 | 282 |
5Ni5RuZSM-5 | 306 | 0.180 | 0.103 | 250 |
10Ni5RuZSM-5 | 215 | 0.162 | 0.065 | 161 |
Samples | O (at.%) | Si (at.%) | Ni (at.%) | Al (at.%) | Ru (at.%) |
---|---|---|---|---|---|
10NiZSM-5 | 58.5 | 32.2 | 3.9 | 5.4 | - |
5RuZSM-5 | 59.5 | 35.8 | - | 2.7 | 2.0 |
10Ni5RuZSM-5 | 54.0 | 29.1 | 6.8 | 8.9 | 1.2 |
Sample | CH4 Selectivity, % |
---|---|
5NiZSM-5 | 20 |
10NiZSM-5 | 19 |
5RuZSM-5 | 25 |
5Ni5RuZSM-5 | 29 |
10Ni5RuZSM-5 | 31 |
Catalysts | Reaction Conditions | Catalytic Activity, % | Reference |
---|---|---|---|
Ni/SiO2 | T = 350 °C; 5 wt.% Ni; GHSV = 15,000 mL gcat−1 h−1 | X = 64.7%; SCH4 = 97.5% | [25] |
Ni-Rh/Al2O3 | T = 400 °C; 3.1 wt.% Ni; 0.5 wt.% Rh; GHSV = 60,000 mL gcat−1 h−1 | X = 65%; SCH4 = 95% | [26] |
Ni-Co/Al2O3 | T = 350 °C; 10 wt.% Ni; 10 wt.% Co; GHSV = 133,000 mL gcat−1 h−1 | X = 61.5%; SCH4 = 95% | [27] |
Ni-Ru/Al2O3 | T = 400 °C; 10 wt.% Ni; 1 wt.% Ru; GHSV = 9000 mL gcat−1 h−1 | X = 82%; SCH4 = 100% | [18] |
Ru-Ni/CeZr | T = 400 °C; 15 wt.% Ni; 1 wt.% Ru; GHSV = 24,000 mL gcat−1 h−1 | X = 62%; SCH4 = 90% | [28] |
Ni-Ru/ZSM-5 | T = 400 °C; 10 wt.% Ni; 5 wt.% Ru; GHSV = 30,000 mL gcat−1 h−1 | X = 82%; SCH4 = 100% | This work |
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Popova, M.; Oykova, M.; Dimitrov, M.; Karashanova, D.; Kovacheva, D.; Atanasova, G.; Szegedi, Á. CO2 Hydrogenation to Renewable Methane on Ni/Ru Modified ZSM-5 Zeolites: The Role of the Preparation Procedure. Catalysts 2022, 12, 1648. https://doi.org/10.3390/catal12121648
Popova M, Oykova M, Dimitrov M, Karashanova D, Kovacheva D, Atanasova G, Szegedi Á. CO2 Hydrogenation to Renewable Methane on Ni/Ru Modified ZSM-5 Zeolites: The Role of the Preparation Procedure. Catalysts. 2022; 12(12):1648. https://doi.org/10.3390/catal12121648
Chicago/Turabian StylePopova, Margarita, Manuela Oykova, Momtchil Dimitrov, Daniela Karashanova, Daniela Kovacheva, Genoveva Atanasova, and Ágnes Szegedi. 2022. "CO2 Hydrogenation to Renewable Methane on Ni/Ru Modified ZSM-5 Zeolites: The Role of the Preparation Procedure" Catalysts 12, no. 12: 1648. https://doi.org/10.3390/catal12121648