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

Xiaofei Zhang, Lixin Chen, Jin Yun, Xiaodong Wang (Corresponding Author), Jie Kong (Corresponding Author)

Research output: Contribution to journalArticle

15 Citations (Scopus)
5 Downloads (Pure)

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 languageEnglish
Pages (from-to)10986-10997
Number of pages12
JournalJournal of Materials Chemistry A
Volume5
Issue number22
Early online date26 Apr 2017
DOIs
Publication statusPublished - Jun 2017

Fingerprint

Microspheres
Nitrobenzenes
Hydrosilylation
Environmental Pollutants
Temperature
Nitrobenzene
Reusability
Precious metals
Nanostructured materials
Discrete Fourier transforms
Specific surface area
X ray powder diffraction
Nanocrystals
Catalysis
Fourier transform infrared spectroscopy
Catalyst activity
Magnetic properties
Pyrolysis
Carbon
X ray photoelectron spectroscopy

Cite this

Constructing magnetic Si-C-Fe hybrid microspheres for room temperature nitroarenes reduction. / Zhang, Xiaofei ; Chen, Lixin; Yun, Jin ; Wang, Xiaodong (Corresponding Author); Kong, Jie (Corresponding Author).

In: Journal of Materials Chemistry A, Vol. 5, No. 22, 06.2017, p. 10986-10997.

Research output: Contribution to journalArticle

Zhang, Xiaofei ; Chen, Lixin ; Yun, Jin ; Wang, Xiaodong ; Kong, Jie . / Constructing magnetic Si-C-Fe hybrid microspheres for room temperature nitroarenes reduction. In: Journal of Materials Chemistry A. 2017 ; Vol. 5, No. 22. pp. 10986-10997.
@article{7dc1ef7baa1244c285e0682b0d55b350,
title = "Constructing magnetic Si-C-Fe hybrid microspheres for room temperature nitroarenes reduction",
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.",
author = "Xiaofei Zhang and Lixin Chen and Jin Yun and Xiaodong Wang and Jie Kong",
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.",
year = "2017",
month = "6",
doi = "10.1039/C7TA01156C",
language = "English",
volume = "5",
pages = "10986--10997",
journal = "Journal of Materials Chemistry A",
issn = "2050-7488",
publisher = "Royal Society of Chemistry (Great Britain)",
number = "22",

}

TY - JOUR

T1 - Constructing magnetic Si-C-Fe hybrid microspheres for room temperature nitroarenes reduction

AU - Zhang, Xiaofei

AU - Chen, Lixin

AU - Yun, Jin

AU - Wang, Xiaodong

AU - Kong, Jie

N1 - 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.

PY - 2017/6

Y1 - 2017/6

N2 - 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.

AB - 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.

U2 - 10.1039/C7TA01156C

DO - 10.1039/C7TA01156C

M3 - Article

VL - 5

SP - 10986

EP - 10997

JO - Journal of Materials Chemistry A

JF - Journal of Materials Chemistry A

SN - 2050-7488

IS - 22

ER -