Abstract
In this work, we present the first synthesis and characterization of magnetic Si-C-Fe hybrid microspheres and their catalysis in room temperature reduction of 4-nitrophenol as a representative sustainable process of 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 PDVB surface and 1, 1’-bis (dimethylsilyl)ferrocene, where further pyrolysis led to the formation of α-Fe nanocrystals-containing Si-C-Fe hybrid microspheres. The precursor and hybrid microspheres were characterized in terms of 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, 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 performance outperforms 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.
Original language | English |
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Pages (from-to) | 10986-10997 |
Number of pages | 12 |
Journal | Journal of Materials Chemistry A |
Volume | 5 |
Issue number | 22 |
Early online date | 26 Apr 2017 |
DOIs | |
Publication status | Published - Jun 2017 |
Bibliographical note
This research is supported by the National Natural Science Foundation of China(21174112). X.W. acknowledges support from School of Engineering, the University
of Aberdeen. The useful discussion with Dr. M.D. Symes (University of Glasgow) is
gratefully acknowledged.