Cobalt nanoclusters coated with N-doped carbon for chemoselective nitroarene hydrogenation and tandem reactions in water

Autor: Pascual Oña-Burgos, Sergio Rojas-Buzo, Silvia Gutiérrez-Tarriño, José J. Calvino, Giovanni Agostini, Christian W. Lopes, Avelino Corma
Přispěvatelé: Ministerio de Economía y Competitividad (España)
Rok vydání: 2021
Předmět:
Zdroj: Digital.CSIC. Repositorio Institucional del CSIC
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ISSN: 1463-9270
1463-9262
DOI: 10.1039/d1gc00706h
Popis: The development of active and selective non-noble metal-based catalysts for the chemoselective reduction of nitro compounds in aquo media under mild conditions is an attractive research area. Herein, the synthesis of subnanometric and stable cobalt nanoclusters, covered by N-doped carbon layers as core-shell (Co@NC-800), for the chemoselective reduction of nitroarenes is reported. TheCo@NC-800catalyst was prepared by the pyrolysis of the Co(tpy)complex impregnated on Vulcan carbon. In fact, the use of a molecular complex based on six N-Co bonds drives the formation of a well-defined and distributed cobalt core-shell nanocluster covered by N-doped carbon layers. In order to elucidate its nature, it has been fully characterized by using several advanced techniques. In addition, this as-prepared catalyst showed high activity, chemoselectivity and stability toward the reduction of nitro compounds with Hand under mild reaction conditions; water was used as a green solvent, improving the previous results based on cobalt catalysts. Moreover, theCo@NC-800catalyst is also active and selective for the one-pot synthesis of secondary aryl amines and isoindolinones through the reductive amination of nitroarenes. Finally, based on diffraction and spectroscopic studies, metallic cobalt nanoclusters with surface CoNpatches have been proposed as the active phase in theCo@NC-800material.
The authors acknowledge the financial support from the Spanish Government (RTI2018-096399-A-I00) and the Program Severo Ochoa SEV-2016-0683. S. G. T. is thankful to MINECO for her FPU Ph.D. contract FPU16/02117. P. O.-B. is thankful to MICCIN for his Ramón y Cajal contract RYC-2014-16620 and to UPV for the grant PAID-06-18/SP20180172The High-Resolution STEM data were recorded at the DME-UCA node of the ELECMI ICTS Spanish National Infrastructure for Electron Microscopy of Materials. JJC acknowledges financial support from MINECO/FEDER (Project MAT2017-97579-R). C. W. L. acknowledges the Visiting Researcher Fellowship from PRH 50.1 – ANP/FINEP Human Resources Program (Brazil).
Databáze: OpenAIRE