Dry Reforming of Methane on Ni/Nanorod-CeO<sub>2</sub> Catalysts Prepared by One-Pot Hydrothermal Synthesis: The Effect of Ni Content on Structure, Activity, and Stability
The nanorod morphology of the CeO<sub>2</sub> support has been recognized as more beneficial than other morphologies for catalytic activity in the dry reforming of methane. Ni/nanorod-CeO<sub>2</sub> catalysts with different Ni contents were prepared by one-pot hydrothermal s...
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MDPI AG
2022-06-01
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| Online Access: | https://www.mdpi.com/2624-781X/3/3/25 |
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| author | Simonetta Tuti Igor Luisetto Umberto Pasqual Laverdura Eleonora Marconi |
| author_facet | Simonetta Tuti Igor Luisetto Umberto Pasqual Laverdura Eleonora Marconi |
| author_sort | Simonetta Tuti |
| collection | DOAJ |
| description | The nanorod morphology of the CeO<sub>2</sub> support has been recognized as more beneficial than other morphologies for catalytic activity in the dry reforming of methane. Ni/nanorod-CeO<sub>2</sub> catalysts with different Ni contents were prepared by one-pot hydrothermal synthesis. Samples were characterized by X-ray diffraction (XRD), H<sub>2</sub>-temperature-programmed reduction (H<sub>2</sub>-TPR), H<sub>2</sub>-temperature-programmed desorption (H<sub>2</sub>-TPD), field emission scanning electron microscopy/energy dispersive spectroscopy (FE-SEM/EDS), Brunauer–Emmet–Teller (BET) and Barrett–Joyner–Halenda (BHJ) analysis. The effect of Ni content on the size and the intrinsic strain of ceria was analyzed by the Size–Strain plot and Williamson–Hall plot of XRD data. The average Ni particle size and Ni dispersion were determined by H<sub>2</sub>-TPD. XRD and H<sub>2</sub>-TPR analysis revealed a strong Ni–support interaction that limited nickel sintering. The activity for the dry reforming of methane was tested with the stoichiometric mixture CO<sub>2</sub>:CH<sub>4</sub>:N<sub>2</sub>:He = 20:20:20:140, gas hourly space velocity (GHSV) = 300 L g<sup>−1</sup> h<sup>−1</sup>, and temperatures in the range of 545–800 °C. The turnover frequency (TOF) value increased linearly with the average Ni particle size in the range of 5.5–33 nm, suggesting the structure sensitivity of the reaction. Samples with Ni loading of 4–12 wt.% showed high H<sub>2</sub>/CO selectivity and stability over time on stream, whereas the sample with a Ni loading of 2 wt.% was less selective and underwent rapid deactivation. Only a small amount of nanotubular carbon was observed by FE-SEM after the time-on-stream experiment. Deactivation of the low-Ni-content sample is ascribed to the easier oxidation of the small Ni particles. |
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| language | English |
| last_indexed | 2024-03-09T22:41:03Z |
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| spelling | doaj.art-d7f2071d1b3545e38bacc0153d3d224f2023-11-23T18:40:27ZengMDPI AGReactions2624-781X2022-06-013333335110.3390/reactions3030025Dry Reforming of Methane on Ni/Nanorod-CeO<sub>2</sub> Catalysts Prepared by One-Pot Hydrothermal Synthesis: The Effect of Ni Content on Structure, Activity, and StabilitySimonetta Tuti0Igor Luisetto1Umberto Pasqual Laverdura2Eleonora Marconi3Department of Science, Roma Tre University, Via della Vasca Navale 79, 00146 Rome, ItalyItalian National Agency for New Technologies, Energy and Sustainable Economic Development (ENEA), Via Anguillarese 301, 00123 Rome, ItalyDepartment of Science, Roma Tre University, Via della Vasca Navale 79, 00146 Rome, ItalyDepartment of Science, Roma Tre University, Via della Vasca Navale 79, 00146 Rome, ItalyThe nanorod morphology of the CeO<sub>2</sub> support has been recognized as more beneficial than other morphologies for catalytic activity in the dry reforming of methane. Ni/nanorod-CeO<sub>2</sub> catalysts with different Ni contents were prepared by one-pot hydrothermal synthesis. Samples were characterized by X-ray diffraction (XRD), H<sub>2</sub>-temperature-programmed reduction (H<sub>2</sub>-TPR), H<sub>2</sub>-temperature-programmed desorption (H<sub>2</sub>-TPD), field emission scanning electron microscopy/energy dispersive spectroscopy (FE-SEM/EDS), Brunauer–Emmet–Teller (BET) and Barrett–Joyner–Halenda (BHJ) analysis. The effect of Ni content on the size and the intrinsic strain of ceria was analyzed by the Size–Strain plot and Williamson–Hall plot of XRD data. The average Ni particle size and Ni dispersion were determined by H<sub>2</sub>-TPD. XRD and H<sub>2</sub>-TPR analysis revealed a strong Ni–support interaction that limited nickel sintering. The activity for the dry reforming of methane was tested with the stoichiometric mixture CO<sub>2</sub>:CH<sub>4</sub>:N<sub>2</sub>:He = 20:20:20:140, gas hourly space velocity (GHSV) = 300 L g<sup>−1</sup> h<sup>−1</sup>, and temperatures in the range of 545–800 °C. The turnover frequency (TOF) value increased linearly with the average Ni particle size in the range of 5.5–33 nm, suggesting the structure sensitivity of the reaction. Samples with Ni loading of 4–12 wt.% showed high H<sub>2</sub>/CO selectivity and stability over time on stream, whereas the sample with a Ni loading of 2 wt.% was less selective and underwent rapid deactivation. Only a small amount of nanotubular carbon was observed by FE-SEM after the time-on-stream experiment. Deactivation of the low-Ni-content sample is ascribed to the easier oxidation of the small Ni particles.https://www.mdpi.com/2624-781X/3/3/25CO<sub>2</sub> recyclingdry reforming of methaneDRMceria nanorod morphologyNi/nanorod-CeO<sub>2</sub> catalystH<sub>2</sub>-TPD analysis of nickel dispersion |
| spellingShingle | Simonetta Tuti Igor Luisetto Umberto Pasqual Laverdura Eleonora Marconi Dry Reforming of Methane on Ni/Nanorod-CeO<sub>2</sub> Catalysts Prepared by One-Pot Hydrothermal Synthesis: The Effect of Ni Content on Structure, Activity, and Stability Reactions CO<sub>2</sub> recycling dry reforming of methane DRM ceria nanorod morphology Ni/nanorod-CeO<sub>2</sub> catalyst H<sub>2</sub>-TPD analysis of nickel dispersion |
| title | Dry Reforming of Methane on Ni/Nanorod-CeO<sub>2</sub> Catalysts Prepared by One-Pot Hydrothermal Synthesis: The Effect of Ni Content on Structure, Activity, and Stability |
| title_full | Dry Reforming of Methane on Ni/Nanorod-CeO<sub>2</sub> Catalysts Prepared by One-Pot Hydrothermal Synthesis: The Effect of Ni Content on Structure, Activity, and Stability |
| title_fullStr | Dry Reforming of Methane on Ni/Nanorod-CeO<sub>2</sub> Catalysts Prepared by One-Pot Hydrothermal Synthesis: The Effect of Ni Content on Structure, Activity, and Stability |
| title_full_unstemmed | Dry Reforming of Methane on Ni/Nanorod-CeO<sub>2</sub> Catalysts Prepared by One-Pot Hydrothermal Synthesis: The Effect of Ni Content on Structure, Activity, and Stability |
| title_short | Dry Reforming of Methane on Ni/Nanorod-CeO<sub>2</sub> Catalysts Prepared by One-Pot Hydrothermal Synthesis: The Effect of Ni Content on Structure, Activity, and Stability |
| title_sort | dry reforming of methane on ni nanorod ceo sub 2 sub catalysts prepared by one pot hydrothermal synthesis the effect of ni content on structure activity and stability |
| topic | CO<sub>2</sub> recycling dry reforming of methane DRM ceria nanorod morphology Ni/nanorod-CeO<sub>2</sub> catalyst H<sub>2</sub>-TPD analysis of nickel dispersion |
| url | https://www.mdpi.com/2624-781X/3/3/25 |
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