A new mixed-linker Fe-MOF as a multifunctional bio-photocatalyst for tandem photo-oxidation condensation reaction
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Título: | A new mixed-linker Fe-MOF as a multifunctional bio-photocatalyst for tandem photo-oxidation condensation reaction |
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Autor/es: | Rouzifar, Majid | Sobhani, Sara | Farrokhi, Alireza | Sansano, Jose M. |
Grupo/s de investigación o GITE: | Síntesis Asimétrica (SINTAS) |
Centro, Departamento o Servicio: | Universidad de Alicante. Departamento de Química Orgánica | Universidad de Alicante. Instituto Universitario de Síntesis Orgánica |
Palabras clave: | Tandem | Photocatalyst | Sunlight irradiation | Multifunctional catalyst | Mixed-linker | Triarylpyridine |
Fecha de publicación: | 13-oct-2023 |
Editor: | Elsevier |
Cita bibliográfica: | Journal of Photochemistry and Photobiology A: Chemistry. 2024, 447: 115263. https://doi.org/10.1016/j.jphotochem.2023.115263 |
Resumen: | A novel mixed-linker of iron-based metal–organic frameworks named Fe(INA)(H2N-BDC) has been directly synthesized by mixing 2-amino-1,4-benzenedicarboxylic acid (NH2-BDC) and isonicotinic acid (INA) using hydrothermal method. Its characterization was fully performed by a number of methods such as FT-IR, PXRD, XPS, FESEM, TEM, TGA, ICP and BET and used as a multifunctional bio-photocatalyst for the preparation of 2,4,6-triarylpyridines (TAPs) via tandem photo-oxidation condensation reactions starting from alcohols under sunlight irradiation and air atmosphere in ethanol. Mixed-linker Fe-MOF showed enhanced catalytic activity compared with its analogues with one single ligand, which indicates the synergistic effect of two linkers and Fe-O clusters in Fe(INA)(H2N-BDC) as a photocatalyst with lower band gap. This observation confirmed by an important reduction in the band gap energy and a rise in the characteristic emission of mixed-linker Fe-MOF compared with Fe-MIL-101-NH2 according to the DRS analysis and fluorescence spectrophotometry, respectively. EPR studies clearly indicated that Fe(INA)(H2N-BDC) produces 1O2 and O2•- as active oxygen units under sunlight illumination. Moreover, amine groups in NH2-BDC provide basic functional groups, which in cooperation with acidic sites (Fe in the metal nodes) promote the condensation of the in-situ formed aldehydes with acetophenone and ammonium acetate. Using sunlight irradiation as an energy-saving source, air as a safe oxidant, good yields, reusability of the photocatalyst and any requirement of additives make the present method as an environmentally-friendly method for the preparation of these important scaffolds. This is the first report of the synthesis of TAPs starting from alcohols catalyzed by MOFs. |
Patrocinador/es: | We thank University of Birjand Research Council for supporting of this work, Spanish Ministerio de Economía, Industria y Competitividad, Agencia Estatal de Investigación (AEI) and Fondo Europeo de Desarrollo Regional (FEDER, EU) (PID2019-107268GB-I00), University of Alicante for the access to the FESEM, EDX, mapping, TEM, XPS and N2 absorption-desorption facilities, and also Prof. Hermenegildo García form Universitat Politecnica de Valencia for the EPR analysis. |
URI: | http://hdl.handle.net/10045/138050 |
ISSN: | 1010-6030 (Print) | 1873-2666 (Online) |
DOI: | 10.1016/j.jphotochem.2023.115263 |
Idioma: | eng |
Tipo: | info:eu-repo/semantics/article |
Derechos: | © 2023 Elsevier B.V. |
Revisión científica: | si |
Versión del editor: | https://doi.org/10.1016/j.jphotochem.2023.115263 |
Aparece en las colecciones: | INV - SINTAS - Artículos de Revistas |
Archivos en este ítem:
Archivo | Descripción | Tamaño | Formato | |
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Rouzifar_etal_2023_JPhotochemPhotobiol_final.pdf | Versión final (acceso restringido) | 5,74 MB | Adobe PDF | Abrir Solicitar una copia |
Rouzifar_etal_2023_JPhotochemPhotobiol_accepted.pdf | Embargo 24 meses (acceso abierto: 14 oct. 2025) | 1,89 MB | Adobe PDF | Abrir Solicitar una copia |
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