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Ultrasonic-assisted preparation of ultrafine Pd nanocatalysts loaded on Cl^--intercalated MgAl layered double hydroxides for the catalytic dehydrogenation of dodecahydro-N-ethylcarbazole.

ABSTRACT: 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 CO₃^2- in LDHs interlayer, and promoted PdCl₄^2- 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 PdCl₄^2- 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.

SUBMITTER: Wu Y

PROVIDER: S-EPMC9310112 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:BackgroundTo enhance ocular bioavailability, the traditional strategies have focused on prolonging precorneal retention and improving corneal permeability by nano-carriers with positive charge, thiolated polymer, absorption enhancer and so on. Glycylsarcosine (GS) as an active target ligand of the peptide tranpsporter-1 (PepT-1), could specific interact with the PepT-1 on the cornea and guide the nanoparticles to the treating site.PurposeThe objective of the study was to explore the active targeting intercalated nanocomposites based on chitosan-glutathione-glycylsarcosine (CG-GS) and layered double hydroxides (LDH) as novel carriers for the treatment of mid-posterior diseases.Materials and methodsCG-GS-LDH intercalated nanocomposites were prepared by the coprecipitation hydrothermal method. In vivo precorneal retention study, ex vivo fluorescence images, in vivo experiment for distribution and irritation were studied in rabbits. The cytotoxicity and cellular uptake were studied in human corneal epithelial primary cells (HCEpiC).ResultsCG-GS-LDH nanocomposites were prepared successfully and characterized by FTIR and XRD. Experiments with rabbits showed longer precorneal retention and higher distribution of fluorescence probe/model drug. In vitro cytological study, CG-GS-LDH nanocomposites exhibited enhanced cellular uptake compared to pure drug solution. Furthermore, the investigation of cellular uptake mechanisms demonstrated that both the active transport by PepT-1 and clathrin-mediated endocytosis were involved in the internalization of CG-GS-LDH intercalated nanocomposites. An ocular irritation study and a cytotoxicity test indicated that these nanocomposites produced no significant irritant effects.ConclusionsThe active targeting intercalated nanocomposites could have great potential for topical ocular drug delivery due to the capacity for prolonging the retention on the ocular surface, enhancing the drug permeability through the cornea, and efficiently delivering the drug to the targeted site.

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Ultrasonic-assisted preparation of ultrafine Pd nanocatalysts loaded on Cl--intercalated MgAl layered double hydroxides for the catalytic dehydrogenation of dodecahydro-N-ethylcarbazole.

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Ultrasonic-assisted preparation of ultrafine Pd nanocatalysts loaded on Cl^--intercalated MgAl layered double hydroxides for the catalytic dehydrogenation of dodecahydro-N-ethylcarbazole.