High catalytic activity and selectivity for hydroxylation of benzene to phenol over multi-walled carbon nanotubes supported Fe3O4 catalyst

被引：101

作者：

Song, Shaoqing ^{[1
]}

Yang, Hongxiao ^{[1
]}

Rao, Richuan ^{[1
]}

Liu, Huade ^{[1
]}

Zhang, Aimin ^{[1
]}

机构：

[1] Nanjing Univ, Sch Chem & Chem Engn, MOE, Key Lab Mesoscop Chem, Nanjing 210093, Peoples R China

来源：

APPLIED CATALYSIS A-GENERAL | 2010年 / 375卷 / 02期

基金：

中国国家自然科学基金;

关键词：

Multi-walled carbon nanotubes; Fe3O4; Defects; Hydroxylation of benzene; Phenol; OXIDATION; SIDEWALLS; CONVERSION; MAGNETITE; DEFECTS;

D O I：

10.1016/j.apcata.2010.01.008

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

Multi-walled carbon nanotubes supported Fe3O4 catalysts (Fe/MWCNTs) were prepared for catalyzing the hydroxylation of benzene in the presence of hydrogen peroxide. The iron species in Fe/MWCNTs is Fe3O4 due to the spontaneous reduction of partial Fe3+ on the defect sites of multi-walled carbon nanotubes (MWCNTs), which is different from the Fe2O3 in the active carbon supported iron (Fe/AC) and graphitic carbon supported iron (Fe/GC) catalysts prepared by the same procedure. The benzene conversion was enhanced by 3.5 and 5.4 times, and the selectivity to phenol was increased by 2.1 and 1.5 times over Fe/MWCNTs catalyst in reference to the latter two carbon-based catalysts. The high catalytic activity for Fe/MWCNTs catalyst mainly comes from the more efficient catalytic component of Fe3O4 and the beneficial topology of MWCNTs. The high selectivity to phenol should arise from the consumption of the excessive hydroxyl radicals by MWCNTs, hereby preventing the further oxidation of phenol. The catalytic performance of Fe/MWCNTs is also superior to other carbon-free support-based iron catalysts, such as Fe/gamma-Al2O3, Fe/MCM-41, Fe/HY and Fe/HZSM-5. These results indicate the potential application of Fe/MWCNTs catalyst in the hydroxylation of benzene to phenol. (C) 2010 Elsevier B.V. All rights reserved.

引用

页码：265 / 271

页数：7

共 37 条

[1] Influence of diameter in the Raman spectra of aligned multi-walled carbon nanotubes [J].

Antunes, E. F. ;

Lobo, A. O. ;

Corat, E. J. ;

Trava-Airoldi, V. J. .

CARBON, 2007, 45 (05) :913-921

[2] Characterization methods of carbon nanotubes: a review [J].

Belin, T ;

Epron, F .

MATERIALS SCIENCE AND ENGINEERING B-SOLID STATE MATERIALS FOR ADVANCED TECHNOLOGY, 2005, 119 (02) :105-118

[3] The reactivity of defects at the sidewalls of single-walled carbon nanotubes: The Stone-Wales defect [J].

Bettinger, HF .

JOURNAL OF PHYSICAL CHEMISTRY B, 2005, 109 (15) :6922-6924

[4] Thermogravimetric analysis of the oxidation of multiwalled carbon nanotubes: Evidence for the role of defect sites in carbon nanotube chemistry [J].

Bom, D ;

Andrews, R ;

Jacques, D ;

Anthony, J ;

Chen, BL ;

Meier, MS ;

Selegue, JP .

NANO LETTERS, 2002, 2 (06) :615-619

[5] A photoelectron spectroscopy study of ion-irradiation induced defects in single-wall carbon nanotubes [J].

Chakraborty, Amit K. ;

Woolley, R. A. J. ;

Butenko, Yu. V. ;

Dhanak, V. R. ;

Siller, L. ;

Hunt, M. R. C. .

CARBON, 2007, 45 (14) :2744-2750

[6] Hydroxylation of benzene over TS-PQ™ catalyst [J].

Chammingkwan, P. ;

Hoelderich, W. F. ;

Mongkhonsi, T. ;

Kanchanawanichakul, P. .

APPLIED CATALYSIS A-GENERAL, 2009, 352 (1-2) :1-9

[7] A facile synthesis of palladium nanoparticles supported on functional carbon nanotubes and its novel catalysis for ethanol electrooxidation [J].

Chen, Xiao-mei ;

Lin, Zhi-jie ;

jia, Tian-tian ;

Cai, Zhi-min ;

Huang, Xiao-li ;

Jiang, Ya-qi ;

Chen, Xi ;

Chen, Guo-nan .

ANALYTICA CHIMICA ACTA, 2009, 650 (01) :54-58

[8] Spontaneous reduction of metal ions on the sidewalls of carbon nanotubes [J].

Choi, HC ;

Shim, M ;

Bangsaruntip, S ;

Dai, HJ .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2002, 124 (31) :9058-9059

[9] Direct synthesis of phenol from benzene on iron-impregnated activated carbon catalysts [J].

Choi, JS ;

Kim, TH ;

Choo, KY ;

Sung, JS ;

Saidutta, MB ;

Ryu, SO ;

Song, SD ;

Ramachandra, B ;

Rhee, YW .

APPLIED CATALYSIS A-GENERAL, 2005, 290 (1-2) :1-8

[10] Natural and H2-reduced limonite for organic oxidation by a Fenton-like system:: Mechanism study via ESI-MS and theoretical calculations [J].

de Souza, Wladmir F. ;

Guimaraes, Iara R. ;

Oliveira, Luiz C. A. ;

Guerreiro, Mario C. ;

Guarieiro, Aline L. N. ;

Carvalho, Kele T. G. .

JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 2007, 278 (1-2) :145-151

← 1 2 3 4 →