Ultrasonic-assisted preparation of ultrafine Pd nanocatalysts loaded on Cl−-intercalated MgAl layered double hydroxides for the catalytic dehydrogenation of dodecahydro-N-ethylcarbazole
N-ethylcarbazole/dodecahydro-N-ethylcarbazole (NEC/H12-NEC) is a promising LOHC, and the development of a catalyst with high activity and stability is the key to realizing its reversible hydrogen storage process. In this paper, ultrafine Pd nanocrystalline catalysts (Pd/LDHs-us) supported on Cl--int...
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| Format: | Article |
| Language: | English |
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Elsevier
2022-08-01
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| Series: | Ultrasonics Sonochemistry |
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| Online Access: | http://www.sciencedirect.com/science/article/pii/S1350417722001924 |
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| author | Yanpeng Wu Xiaoran Liu Xuefeng Bai Wei Wu |
| author_facet | Yanpeng Wu Xiaoran Liu Xuefeng Bai Wei Wu |
| author_sort | Yanpeng Wu |
| collection | DOAJ |
| description | N-ethylcarbazole/dodecahydro-N-ethylcarbazole (NEC/H12-NEC) is a promising LOHC, and the development of a catalyst with high activity and stability is the key to realizing its reversible hydrogen storage process. In this paper, ultrafine Pd nanocrystalline catalysts (Pd/LDHs-us) supported on Cl--intercalated MgAl LDHs were prepared by a simple ultrasonic-assisted reduction method and applied in the dehydrogenation of 12H-NEC. In the process of ultrasonic-assisted reduction, the instantaneous high temperature generated by cavitation decomposed part of the CO32– in LDHs interlayer, and promoted PdCl42- to enter the interlayer and become new intercalated ions. At the same time, hydroxyl groups on the surface of LDHs were excited to generate hydrogen radicals (•H) with strong reducibility, which reduced PdCl42- to Pd nanoparticles (PdNPs) in situ. The remaining Cl- ions continued to exist in the interlayer as intercalated ions. The agglomeration of PdNPs was effectively inhibited, and the average particle size was 1.8 nm, which was uniformly dispersed on LDHs, which improved the catalytic activity of Pd/LDHs-us. The coordination between PdNPs and oxygen in the hydroxyl groups on the surface of LDHs improved its catalytic stability. Using Pd/LDHs-us catalyst, the conversion rate of H12-NEC was 100.0 %, and the dehydrogenation efficiency was 99.3 % at 180℃. When the reaction temperature drops to 170℃, the dehydrogenation efficiency can still reach 94.6 %, showing excellent catalytic performance. The study of dehydrogenation kinetics shows that the apparent activation energy of Pd/LDHs-us catalyst is only 90.97 kJ/mol. This provides a new method and idea for the preparation of efficient dehydrogenation catalysts in the future. |
| first_indexed | 2024-12-11T23:39:14Z |
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| id | doaj.art-e1d91c67ef634170899ce77a7e7c348c |
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| issn | 1350-4177 |
| language | English |
| last_indexed | 2024-12-11T23:39:14Z |
| publishDate | 2022-08-01 |
| publisher | Elsevier |
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| series | Ultrasonics Sonochemistry |
| spelling | doaj.art-e1d91c67ef634170899ce77a7e7c348c2022-12-22T00:45:47ZengElsevierUltrasonics Sonochemistry1350-41772022-08-0188106097Ultrasonic-assisted preparation of ultrafine Pd nanocatalysts loaded on Cl−-intercalated MgAl layered double hydroxides for the catalytic dehydrogenation of dodecahydro-N-ethylcarbazoleYanpeng Wu0Xiaoran Liu1Xuefeng Bai2Wei Wu3National Center for International Research on Catalytic Technology, Key Laboratory of Functional Inorganic Material Chemistry (Ministry of Education), School of Chemistry and Material Sciences, Heilongjiang University, Harbin 150080, ChinaNational Center for International Research on Catalytic Technology, Key Laboratory of Functional Inorganic Material Chemistry (Ministry of Education), School of Chemistry and Material Sciences, Heilongjiang University, Harbin 150080, ChinaNational Center for International Research on Catalytic Technology, Key Laboratory of Functional Inorganic Material Chemistry (Ministry of Education), School of Chemistry and Material Sciences, Heilongjiang University, Harbin 150080, China; Institute of Petrochemistry, Heilongjiang Academy of Sciences, Harbin 150040, China; Corresponding authors.National Center for International Research on Catalytic Technology, Key Laboratory of Functional Inorganic Material Chemistry (Ministry of Education), School of Chemistry and Material Sciences, Heilongjiang University, Harbin 150080, China; Corresponding authors.N-ethylcarbazole/dodecahydro-N-ethylcarbazole (NEC/H12-NEC) is a promising LOHC, and the development of a catalyst with high activity and stability is the key to realizing its reversible hydrogen storage process. In this paper, ultrafine Pd nanocrystalline catalysts (Pd/LDHs-us) supported on Cl--intercalated MgAl LDHs were prepared by a simple ultrasonic-assisted reduction method and applied in the dehydrogenation of 12H-NEC. In the process of ultrasonic-assisted reduction, the instantaneous high temperature generated by cavitation decomposed part of the CO32– in LDHs interlayer, and promoted PdCl42- to enter the interlayer and become new intercalated ions. At the same time, hydroxyl groups on the surface of LDHs were excited to generate hydrogen radicals (•H) with strong reducibility, which reduced PdCl42- to Pd nanoparticles (PdNPs) in situ. The remaining Cl- ions continued to exist in the interlayer as intercalated ions. The agglomeration of PdNPs was effectively inhibited, and the average particle size was 1.8 nm, which was uniformly dispersed on LDHs, which improved the catalytic activity of Pd/LDHs-us. The coordination between PdNPs and oxygen in the hydroxyl groups on the surface of LDHs improved its catalytic stability. Using Pd/LDHs-us catalyst, the conversion rate of H12-NEC was 100.0 %, and the dehydrogenation efficiency was 99.3 % at 180℃. When the reaction temperature drops to 170℃, the dehydrogenation efficiency can still reach 94.6 %, showing excellent catalytic performance. The study of dehydrogenation kinetics shows that the apparent activation energy of Pd/LDHs-us catalyst is only 90.97 kJ/mol. This provides a new method and idea for the preparation of efficient dehydrogenation catalysts in the future.http://www.sciencedirect.com/science/article/pii/S1350417722001924Ultrasonic-assisted reductionCl--intercalated LDHsHydrogen radical reduction in situUltrafine PdNPsDodecahydro-N-ethylcarbazole dehydrogenation |
| spellingShingle | Yanpeng Wu Xiaoran Liu Xuefeng Bai Wei Wu Ultrasonic-assisted preparation of ultrafine Pd nanocatalysts loaded on Cl−-intercalated MgAl layered double hydroxides for the catalytic dehydrogenation of dodecahydro-N-ethylcarbazole Ultrasonics Sonochemistry Ultrasonic-assisted reduction Cl--intercalated LDHs Hydrogen radical reduction in situ Ultrafine PdNPs Dodecahydro-N-ethylcarbazole dehydrogenation |
| title | Ultrasonic-assisted preparation of ultrafine Pd nanocatalysts loaded on Cl−-intercalated MgAl layered double hydroxides for the catalytic dehydrogenation of dodecahydro-N-ethylcarbazole |
| title_full | Ultrasonic-assisted preparation of ultrafine Pd nanocatalysts loaded on Cl−-intercalated MgAl layered double hydroxides for the catalytic dehydrogenation of dodecahydro-N-ethylcarbazole |
| title_fullStr | Ultrasonic-assisted preparation of ultrafine Pd nanocatalysts loaded on Cl−-intercalated MgAl layered double hydroxides for the catalytic dehydrogenation of dodecahydro-N-ethylcarbazole |
| title_full_unstemmed | Ultrasonic-assisted preparation of ultrafine Pd nanocatalysts loaded on Cl−-intercalated MgAl layered double hydroxides for the catalytic dehydrogenation of dodecahydro-N-ethylcarbazole |
| title_short | Ultrasonic-assisted preparation of ultrafine Pd nanocatalysts loaded on Cl−-intercalated MgAl layered double hydroxides for the catalytic dehydrogenation of dodecahydro-N-ethylcarbazole |
| title_sort | ultrasonic assisted preparation of ultrafine pd nanocatalysts loaded on cl intercalated mgal layered double hydroxides for the catalytic dehydrogenation of dodecahydro n ethylcarbazole |
| topic | Ultrasonic-assisted reduction Cl--intercalated LDHs Hydrogen radical reduction in situ Ultrafine PdNPs Dodecahydro-N-ethylcarbazole dehydrogenation |
| url | http://www.sciencedirect.com/science/article/pii/S1350417722001924 |
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