Positive influence of minute Pt addition on the activity of Ni supported on defective graphene for hydrogenation/dehydrogenation of N-ethylcarbazole as liquid organic carrier
Ni nanoparticles (≈ 8 nm) have been prepared at about 15 wt% loading strongly grafted on N-doped graphitic carbon matrix [Ni@(N)C] by pyrolysis of Ni(OAc)2 adsorbed on chitosan. Ni@(N)C was used as catalyst for H2 storage/release on N-ethylcarbazole (EC). Ni@(N)C exhibits higher H2 storage capacity...
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| Format: | Article |
| Language: | English |
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Elsevier
2023-04-01
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| Series: | Catalysis Communications |
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| Online Access: | http://www.sciencedirect.com/science/article/pii/S1566736723000432 |
| _version_ | 1797842826832117760 |
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| author | Alberto Garcia-Baldovi Lu Peng Amarajothi Dhakshinamoorthy Abdullah M. Asiri Ana Primo Hermenegildo Garcia |
| author_facet | Alberto Garcia-Baldovi Lu Peng Amarajothi Dhakshinamoorthy Abdullah M. Asiri Ana Primo Hermenegildo Garcia |
| author_sort | Alberto Garcia-Baldovi |
| collection | DOAJ |
| description | Ni nanoparticles (≈ 8 nm) have been prepared at about 15 wt% loading strongly grafted on N-doped graphitic carbon matrix [Ni@(N)C] by pyrolysis of Ni(OAc)2 adsorbed on chitosan. Ni@(N)C was used as catalyst for H2 storage/release on N-ethylcarbazole (EC). Ni@(N)C exhibits higher H2 storage capacity than analogous Ni nanoparticles (NPs) supported on silica. The addition of minute amounts (18 ppm) of Pt increases significantly the H2 storage/release activity of Ni@(N)C due to effect of Pt promoting H spill over the Ni NPs. There is no linear correlation between Pt concentration and hydrogenation/dehydrogenation activity of Ni@(N)C, the lowest Pt loading (18 ppm) resulting in the most efficient Pt/Ni@(N)C for hydrogenation-dehydrogenation of EC. This fact was attributed to the presence of small Pt clusters or single atoms, while higher concentration would correspond to a less-efficient larger cluster regime. The most efficient Pt/Ni@(N)C-18 catalyst was used for four consecutive hydrogenation/dehydrogenation cycles, exhibiting some fatigue in the H2 storage/release of the same EC batch that was attributed to the increase in the product mixture complexity upon cycling, with the formation of some intermediates that undergo more difficult hydrogenation/dehydrogenation reaction as well as partial catalyst deactivation. After four cycles, (Pt)Ni@(N)C exhibits in the fifth use a H2 storage capacity of 5.2 wt%, somewhat lower than the 5.8 wt% H2 capacity of the fresh sample, while no changes in the XRD, TEM and XPS characterization of the five-times used catalyst compared to the fresh material is observed. |
| first_indexed | 2024-04-09T16:54:33Z |
| format | Article |
| id | doaj.art-2b6a9ffefa104b0e8c035dee09a1d959 |
| institution | Directory Open Access Journal |
| issn | 1873-3905 |
| language | English |
| last_indexed | 2024-04-09T16:54:33Z |
| publishDate | 2023-04-01 |
| publisher | Elsevier |
| record_format | Article |
| series | Catalysis Communications |
| spelling | doaj.art-2b6a9ffefa104b0e8c035dee09a1d9592023-04-21T06:40:54ZengElsevierCatalysis Communications1873-39052023-04-01177106641Positive influence of minute Pt addition on the activity of Ni supported on defective graphene for hydrogenation/dehydrogenation of N-ethylcarbazole as liquid organic carrierAlberto Garcia-Baldovi0Lu Peng1Amarajothi Dhakshinamoorthy2Abdullah M. Asiri3Ana Primo4Hermenegildo Garcia5Instituto Universitario de Tecnología Química, Consejo Superior de Investigaciones Científicas-Universitat Politecnica de Valencia, Universitat Politecnica de Valencia, Av. De los Naranjos s/n, 46022, Valencia, SpainInstituto Universitario de Tecnología Química, Consejo Superior de Investigaciones Científicas-Universitat Politecnica de Valencia, Universitat Politecnica de Valencia, Av. De los Naranjos s/n, 46022, Valencia, SpainInstituto Universitario de Tecnología Química, Consejo Superior de Investigaciones Científicas-Universitat Politecnica de Valencia, Universitat Politecnica de Valencia, Av. De los Naranjos s/n, 46022, Valencia, SpainCenter of Excellence in Advanced Materials Research, King Abdullaziz University, Jeddah, Saudi ArabiaInstituto Universitario de Tecnología Química, Consejo Superior de Investigaciones Científicas-Universitat Politecnica de Valencia, Universitat Politecnica de Valencia, Av. De los Naranjos s/n, 46022, Valencia, SpainInstituto Universitario de Tecnología Química, Consejo Superior de Investigaciones Científicas-Universitat Politecnica de Valencia, Universitat Politecnica de Valencia, Av. De los Naranjos s/n, 46022, Valencia, Spain; Center of Excellence in Advanced Materials Research, King Abdullaziz University, Jeddah, Saudi Arabia; Corresponding author at: Instituto Universitario de Tecnología Química, Consejo Superior de Investigaciones Científicas-Universitat Politecnica de Valencia, Universitat Politecnica de Valencia, Av. De los Naranjos s/n, 46022, Valencia, Spain.Ni nanoparticles (≈ 8 nm) have been prepared at about 15 wt% loading strongly grafted on N-doped graphitic carbon matrix [Ni@(N)C] by pyrolysis of Ni(OAc)2 adsorbed on chitosan. Ni@(N)C was used as catalyst for H2 storage/release on N-ethylcarbazole (EC). Ni@(N)C exhibits higher H2 storage capacity than analogous Ni nanoparticles (NPs) supported on silica. The addition of minute amounts (18 ppm) of Pt increases significantly the H2 storage/release activity of Ni@(N)C due to effect of Pt promoting H spill over the Ni NPs. There is no linear correlation between Pt concentration and hydrogenation/dehydrogenation activity of Ni@(N)C, the lowest Pt loading (18 ppm) resulting in the most efficient Pt/Ni@(N)C for hydrogenation-dehydrogenation of EC. This fact was attributed to the presence of small Pt clusters or single atoms, while higher concentration would correspond to a less-efficient larger cluster regime. The most efficient Pt/Ni@(N)C-18 catalyst was used for four consecutive hydrogenation/dehydrogenation cycles, exhibiting some fatigue in the H2 storage/release of the same EC batch that was attributed to the increase in the product mixture complexity upon cycling, with the formation of some intermediates that undergo more difficult hydrogenation/dehydrogenation reaction as well as partial catalyst deactivation. After four cycles, (Pt)Ni@(N)C exhibits in the fifth use a H2 storage capacity of 5.2 wt%, somewhat lower than the 5.8 wt% H2 capacity of the fresh sample, while no changes in the XRD, TEM and XPS characterization of the five-times used catalyst compared to the fresh material is observed.http://www.sciencedirect.com/science/article/pii/S1566736723000432Heterogeneous catalysisLiquid organic hydrogen carriersHydrogen spilloverN-doped graphene as supportPromotional Pt effect |
| spellingShingle | Alberto Garcia-Baldovi Lu Peng Amarajothi Dhakshinamoorthy Abdullah M. Asiri Ana Primo Hermenegildo Garcia Positive influence of minute Pt addition on the activity of Ni supported on defective graphene for hydrogenation/dehydrogenation of N-ethylcarbazole as liquid organic carrier Catalysis Communications Heterogeneous catalysis Liquid organic hydrogen carriers Hydrogen spillover N-doped graphene as support Promotional Pt effect |
| title | Positive influence of minute Pt addition on the activity of Ni supported on defective graphene for hydrogenation/dehydrogenation of N-ethylcarbazole as liquid organic carrier |
| title_full | Positive influence of minute Pt addition on the activity of Ni supported on defective graphene for hydrogenation/dehydrogenation of N-ethylcarbazole as liquid organic carrier |
| title_fullStr | Positive influence of minute Pt addition on the activity of Ni supported on defective graphene for hydrogenation/dehydrogenation of N-ethylcarbazole as liquid organic carrier |
| title_full_unstemmed | Positive influence of minute Pt addition on the activity of Ni supported on defective graphene for hydrogenation/dehydrogenation of N-ethylcarbazole as liquid organic carrier |
| title_short | Positive influence of minute Pt addition on the activity of Ni supported on defective graphene for hydrogenation/dehydrogenation of N-ethylcarbazole as liquid organic carrier |
| title_sort | positive influence of minute pt addition on the activity of ni supported on defective graphene for hydrogenation dehydrogenation of n ethylcarbazole as liquid organic carrier |
| topic | Heterogeneous catalysis Liquid organic hydrogen carriers Hydrogen spillover N-doped graphene as support Promotional Pt effect |
| url | http://www.sciencedirect.com/science/article/pii/S1566736723000432 |
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