MOF-Mediated Synthesis of Supported Fe-Doped Pd Nanoparticles under Mild Conditions for Magnetically Recoverable Catalysis

Open Access

Abstract

[EN] Metal-organic framework (MOF)-driven synthesis is considered as a promising alternative for the development of new catalytic materials with well-designed active sites. This synthetic approach is used here to gradually transform a new bimetallic MOF, with Pd and Fe as the metal components, by the in situ generation of aniline under mild conditions. This methodology results in a compositionally homogeneous nanocomposite formed by Fe-doped Pd nanoparticles that, in turn, are supported on iron oxide-doped carbon. The nanocomposite has been fully characterized by several techniques such as IR and Raman spectroscopy, TEM, XPS, and XAS. The performance of this nanocomposite as an heterogeneous catalyst for hydrogenation of nitroarenes and nitrobenzene coupling with benzaldehyde has been evaluated, proving it to be an efficient and reusable catalyst. ; This work has been supported by the European Union (ERC2016-CoG 724681-S-CAGE), by the Spanish MICINN (Structures of Excellence Severo Ochoa SEV-2016-0683 and Maria de Maeztu CEX2019-000919-M; projects CTQ2017-89528-P, CTQ2015-67592, PGC2018-097277-B-100, and RTI2018-096399A-I00 co-financed by FEDER). We also thank the Generalitat Valenciana (PROMETEO/2018/006 and PROMETEU/2019/066). G.M.E. and P.O.-B. thank MICINN for their "Ramon y Cajal" fellowships. M.G.-M thanks support of a fellowship from "la Caixa" Foundation (LCF/BQ/PI19/11690022) and Generalitat Valenciana (SEJI/2020/036). J.M. thanks MICINN for his PhD fellowship (CTQ2015-67592). The authors also thank the Electron Microscopy Service of Universitat Politicnica de Val~ncia for their support, M. P. Romero for her assistance with TEM measurements and Prof. E. Rodr~guez-Castellin for discussions on the XPS spectra interpretation. This research used resources of the Advanced Photon Source, an Office of Science User Facility operated for the U.S. Department of Energy (DOE) Office of Science by Argonne National Laboratory and was supported by the U.S. DOE under contract no. DE-AC02-06CH11357, and the Canadian ...