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Constructing magnetic Si–C–Fe hybrid microspheres for room temperature nitroarenes reduction

Author:
Zhang, Xiaofei, Chen, Lixin, Yun, Jin, Wang, Xiaodong, Kong, Jie
Source:
Journal of materials chemistry A 2017 v.5 no.22 pp. 10986-10997
ISSN:
2050-7496
Subject:
Fourier transform infrared spectroscopy, X-ray diffraction, X-ray photoelectron spectroscopy, ambient temperature, aminophenols, carbon, catalysts, catalytic activity, iron, magnetic properties, magnetism, microparticles, moieties, nanomaterials, nitrobenzenes, nuclear magnetic resonance spectroscopy, p-nitrophenol, pollutants, porosity, pyrolysis, surface area, transmission electron microscopy
Abstract:
In this work, we present, for the first time, the synthesis and characterization of magnetic Si–C–Fe hybrid microspheres and their catalytic performance in room temperature reduction of 4-nitrophenol as a representative sustainable process for converting environmental pollutants to fine chemicals. The ferrocene-modified polydivinylbenzene (Fc-PDVB) precursor was synthesized by Pt-catalyzed hydrosilylation between the residual vinyl groups on the PDVB surface and 1,1′-bis (dimethylsilyl)ferrocene, where further pyrolysis led to the formation of Fe nanocrystal-containing Si–C–Fe hybrid microspheres. The precursor and hybrid microspheres were characterized by transmission electron microscopy (TEM), Fourier transform infrared spectroscopy (FT-IR), BET surface area/porosity, powder X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), magnetic properties and MAS solid-state NMR measurements. The ultimate microspherical catalyst exhibited nano- and meso-pores, a high specific surface area (i.e., 347.9 m² g⁻¹) and good ferromagnetic properties. Efficient catalytic activity (TOF: 0.163 s⁻¹), 100% selectivity (to 4-aminophenol) and excellent reusability (with easy separation) have been delivered. The achieved microspheres outperform a number of nanomaterials such as supported noble metal particles, composites, monoliths and sheets. We have confirmed by DFT calculations that the activation of 4-nitrophenol via its weak non-covalent interaction with the sp² carbon domain of Si–C–Fe hybrid microspheres contributed to the superior performance which can be extended to a range of nitrobenzenes.
Agid:
6425162