New hybrid materials based on the grafting of Pd(II)-amino complexes on the graphitic surface of AC: preparation, structures and catalytic properties
| Autor: | M.D. Gutierrez-Valero, Rafael López-Garzón, Concepción Salinas-Martínez de Lecea, M. Luz Godino-Salido, F. Javier López-Garzón, Antonio Santiago-Medina, Víctor K. Abdelkader-Fernández, Paloma Arranz-Mascarós, Manuel Melguizo, María Domingo-García, M. Carmen Román-Martínez |
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| Přispěvatelé: | Universidad de Alicante. Departamento de Química Inorgánica, Universidad de Alicante. Instituto Universitario de Materiales, Materiales Carbonosos y Medio Ambiente |
| Rok vydání: | 2016 |
| Předmět: |
General Chemical Engineering
Nanoparticle Nanotechnology 02 engineering and technology 010402 general chemistry 01 natural sciences Catalysis chemistry.chemical_compound Adsorption Polymer chemistry medicine Moiety Química Inorgánica Grafting Pd(II)-amino complexes Chemistry Ligand General Chemistry 021001 nanoscience & nanotechnology AC 0104 chemical sciences Methanol Hybrid materials 0210 nano-technology Hybrid material Graphitic surface Activated carbon medicine.drug |
| Zdroj: | RUA. Repositorio Institucional de la Universidad de Alicante Universidad de Alicante (UA) |
| Popis: | A novel procedure for the preparation of solid Pd(II)-based catalysts consisting of the anchorage of designed Pd(II)-complexes on an activated carbon (AC) surface is reported. Two molecules of the Ar–S–F type (where Ar is a plane-pyrimidine moiety, F a Pd(II)-ligand and S an aliphatic linker) differing in F, were grafted on AC by π–π stacking of the Ar moiety and the graphene planes of the AC, thus favouring the retaining of the metal-complexing ability of F. Adsorption of Pd(II) by the AC/Ar–S–F hybrids occurs via Pd(II)-complexation by F. After deep characterization, the catalytic activities of the AC/Ar–S–F/Pd(II) hybrids on the hydrogenation of 1-octene in methanol as a catalytic test were evaluated. 100% conversion to n-octane at T = 323.1 K and P = 15 bar, was obtained with both catalysts and most of Pd(II) was reduced to Pd(0) nanoparticles, which remained on the AC surface. Reusing the catalysts in three additional cycles reveals that the catalyst bearing the F ligand with a larger Pd-complexing ability showed no loss of activity (100% conversion to n-octane) which is assigned to its larger structural stability. The catalyst with the weaker F ligand underwent a progressive loss of activity (from 100% to 79% in four cycles), due to the constant aggregation of the Pd(0) nanoparticles. Milder conditions, T = 303.1 K and P = 1.5 bar, prevent the aggregation of the Pd(0) nanoparticles in this catalyst allowing the retention of the high catalytic efficiency (100% conversion) in four reaction cycles. The supports of the MINECO (projects MAT2014-60104-C2-1-R, MAT2014-60104-C2-2-R and CTM2010-16770), the Autonomous Regional Government (J. de Andalucía, Groups PAIDI FQM273 and RNM342), the Programa de Fortalecimiento de la I+D+I from UGR and Feder funds and the University of Jaén (Project UJA2014/02_FT/06 corresponding to the PROGRAMA OPERATIVO FEDER ANDALUCÍA) are acknowledged. |
| Databáze: | OpenAIRE |
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