Pd supported on mixed metal oxide as an efficient catalyst for the reductive amination of bio-derived acetol to 2-methylpiperazine
| Autor: | Marcelo Eduardo Domine, Patricia Concepción, Jaime Mazarío, Zaher Raad, Cristina Cerdá-Moreno |
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| Jazyk: | angličtina |
| Rok vydání: | 2020 |
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| Zdroj: | RiuNet. Repositorio Institucional de la Universitat Politécnica de Valéncia instname |
| Popis: | [EN] An efficient process for synthesizing a high added-value N-heterocycle (2-methylpiperazine, 2-MP) via reductive amination of hydroxyacetone or acetol (product of the selective dehydration of glycerol) with ethylenediamine by using Pd supported catalysts under mild reaction conditions is here presented. Catalysts based on Pd nanoparticles supported on metallic oxides and mixed oxides were prepared and characterized by ICP analysis, XRD, HR-TEM, and NH3-TPD, among others. Catalytic activity comparisons of Pd-based materials (also including commercial references) were done and obtained results correlated with metal particle morphology (analyzed by CO-FTIR) and its ability to activate the C = N bond. The best results were attained with Pd/TiO2-Al2O3 and Pd/ZrO2-Al2O3, the former yielding >80% of 2-MP. The Pd/TiO2-Al2O3 catalyst successfully enables the activation of the imine group (C = N), due to a larger number of unsaturated Pd sites in its nanoparticles, while keeping a suitable acidity to effectively and selectively carry out the reductive cyclo-amination reaction even with lower catalyst loadings. This research work offers a new and sustainable catalytic route for the synthesis of organo-nitrogen compounds taking advantage of renewable raw materials (i.e. acetol) as a carbon source and using efficient Pd supported catalysts. The authors express their gratitude to the Spanish Government for the funding (MICINN: CTQ2015-67592, PGC2018-097277-B-I00 and Severo Ochoa Program: SEV-2016-0683). J. M. thanks the MICINN (CTQ2015-67592) for his PhD scholarship. Z. R. thanks the Islamic Center Association for Guidance and Higher Education for his PhD scholarship. The authors also thank the Electron Microscopy Service of Universitat Politecnica de Valencia for their support and M. Parreno-Romero for her assistance with the measurements. |
| Databáze: | OpenAIRE |
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