Journal Home > Volume 4 , Issue 1

Highly ordered mesoporous carbon-alumina nanocomposites (OMCA) have been synthesized for the first time by a multi-component co-assembly method followed by pyrolysis at high temperatures. In this synthesis, resol phenol-formaldehyde resin (PF resin) and alumina sol were respectively used as the carbon and alumina precursors and triblock copolymer Pluronic F127 as the template. N2-adsorption measurements, X-ray diffraction, and transmission electron microscopy revealed that, with an increase of the alumina content in the nanocomposite from 11 to 48 wt.%, the pore size increased from 2.9 to 5.0 nm while the ordered mesoporous structure was retained. Further increasing the alumina content to 53 wt.% resulted in wormhole-like structures, although the pore size distribution was still narrow. The nanocomposite walls are composed of continuous carbon and amorphous alumina, which allows the ordered mesostructure to be well preserved even after the removal of alumina by HF etching or the removal of carbon by calcination in air. The OMCA nanocomposites exhibited good thermostability below 1000 ℃; at higher temperatures the ordered mesostructure partially collapsed, associated with a phase transformation from amorphous alumina into γ-Al2O3. OMCA-supported Pt catalysts exhibited excellent performance in the one-pot transformation of cellulose into hexitols thanks to the unique surface properties of the nanocomposite.


menu
Abstract
Full text
Outline
Electronic supplementary material
About this article

Synthesis, Characterization, and Catalytic Application of Highly Ordered Mesoporous Alumina–Carbon Nanocomposites

Show Author's information Jinming Xu1,2Aiqin Wang1Xiaodong Wang1Dangsheng Su3Tao Zhang1( )
State Key Laboratory of CatalysisDalian Institute of Chemical PhysicsChinese Academy of Sciences, 457 Zhongshan RoadDalian116023China
Graduate University of the Chinese Academy of SciencesBeijing100049China
Fritz-Haber Institute of the Max Planck SocietyBerlinD-14195Germany

Abstract

Highly ordered mesoporous carbon-alumina nanocomposites (OMCA) have been synthesized for the first time by a multi-component co-assembly method followed by pyrolysis at high temperatures. In this synthesis, resol phenol-formaldehyde resin (PF resin) and alumina sol were respectively used as the carbon and alumina precursors and triblock copolymer Pluronic F127 as the template. N2-adsorption measurements, X-ray diffraction, and transmission electron microscopy revealed that, with an increase of the alumina content in the nanocomposite from 11 to 48 wt.%, the pore size increased from 2.9 to 5.0 nm while the ordered mesoporous structure was retained. Further increasing the alumina content to 53 wt.% resulted in wormhole-like structures, although the pore size distribution was still narrow. The nanocomposite walls are composed of continuous carbon and amorphous alumina, which allows the ordered mesostructure to be well preserved even after the removal of alumina by HF etching or the removal of carbon by calcination in air. The OMCA nanocomposites exhibited good thermostability below 1000 ℃; at higher temperatures the ordered mesostructure partially collapsed, associated with a phase transformation from amorphous alumina into γ-Al2O3. OMCA-supported Pt catalysts exhibited excellent performance in the one-pot transformation of cellulose into hexitols thanks to the unique surface properties of the nanocomposite.

Keywords: carbon, Nanocomposite, alumina, mesoporous, cellulose

References(33)

1

Fukuoka, A.; Dhepe, P. L. Catalytic conversion of cellulose into sugar alcohols. Angew. Chem. Int. Ed. 2006, 45, 5161-5163.

2

Luo, C.; Wang, S.; Liu, H. C. Cellulose conversion into polyols catalyzed by reversibly formed acids and supported ruthenium clusters in hot water. Angew. Chem. Int. Ed. 2007, 46, 7636-7639.

3

Ji, N.; Zhang, T.; Zheng, M. Y.; Wang, A. Q.; Wang, H.; Wang, X. D.; Chen, J. G. G. Direct catalytic conversion of cellulose into ethylene glycol using nickel-promoted tungsten carbide catalysts. Angew. Chem. Int. Ed. 2008, 47, 8510-8513.

4

Ji, N.; Zhang, T.; Zheng, M. Y.; Wang, A. Q.; Wang, H.; Wang, X. D.; Shu, Y. Y.; Stottlemyer, A. L.; Chen, J. G. Catalytic conversion of cellulose into ethylene glycol over supported carbide catalysts. Catal. Today 2009, 147, 77-85.

5

Zhang, Y. H.; Wang, A. Q.; Zhang, T. A new 3D mesoporous carbon replicated from commercial silica as a catalyst support for direct conversion of cellulose into ethylene glycol. Chem. Commun. 2010, 46, 862-864.

6

Zheng, M. Y.; Wang, A. Q.; Ji, N.; Pang, J. F.; Wang, X. D.; Zhang, T. Transition metal-tungsten bimetallic catalysts for the conversion of cellulose into ethylene glycol. ChemSusChem 2010, 3, 63-66.

7

Augustin, R. L. Heterogeneous catalysis for the synthetic chemist; Marcel Dekker, Inc. : New York, 1995.

8

Xia, W. S.; Wan, H. L.; Chen, Y. Cluster model study on the surface interactions of γ-alumina-supported metal oxides. J. Mol. Catal. A 1999, 138, 185-195.

9

Abasov, S. I.; Borovkov, V. Y.; Kazansky, V. B. Infrared and adsorption study of strong metal—support interaction in diluted platinum—alumina catalysts. Catal. Lett. 1992, 15, 269-274.

10

Li, D.; Zhou, H.; Honma, I. Design and synthesis of self-ordered mesoporous nanocomposite through controlled in situ crystallization. Nat. Mater. 2004, 3, 65-72.

11

Lu, A. H.; Li, W.; Hou, Z.; Schüth, F. Molecular level dispersed Pd clusters in the carbon walls of ordered mesoporous carbon as a highly selective alcohol oxidation catalyst. Chem. Commun. 2007, 1038-1040.

12

Liang, C.; Dudney, N. J.; Howe J. Y. Hierarchically structured sulfur carbon nanocomposite material for high-energy lithium battery. Chem. Mater. 2009, 21, 4724-4730.

13

Liu, R. L.; Shi, Y. F.; Wan, Y.; Meng, Y.; Zhang, F. Q.; Gu, D.; Chen, Z. X.; Tu, B.; Zhao, D. Y. Triconstituent co-assembly to ordered mesostructured polymer-silica and carbon-silica nanocomposites and large-pore mesoporous carbons with high surface areas. J. Am. Chem. Soc. 2006, 128, 11652-11662.

14

Lin, H. P.; Chang-Chien, C. Y.; Tang, C. Y.; Lin, C. Y. Synthesis of p6mm hexagonal mesoporous carbons and silicas using Pluronic F127-PF resin polymer blends. Micropor. Mesopor. Mater. 2006, 93, 344-348.

15

Hu, Q. Y.; Kou, R.; Pang, J. B.; Ward, T. L.; Cai, M.; Yang, Z. Z.; Lu, Y. F.; Tang, J. Mesoporous carbon/silica nanocomposite through multi-component assembly. Chem. Commun. 2007, 601-603.

16

Gorka, J.; Jaroniec, M. Incorporation of inorganic nanoparticles into mesoporous carbons synthesized by soft templating. J. Phys. Chem. C 2008, 112, 11657-11660.

17

Jaroniec, M.; Gorka, J.; Choma, J.; Zawislak, A. Synthesis and properties of mesoporous carbons with high loadings of inorganic species. Carbon 2009, 47, 3034-3040.

18

Liu, R.; Ren, Y.; Shi, Y.; Zhang, F.; Zhang, L.; Tu, B.; Zhao, D. Controlled synthesis of ordered mesoporous C-TiO2 nanocomposites with crystalline titania frameworks from organic-inorganic-amphiphilic coassembly. Chem. Mater. 2008, 20, 1140-1146.

19

Choma, J.; Zubrowska, A.; Górka, J.; Jaroniec, M. Soft-templating synthesis of nanoporous carbons with incorporated alumina nanoparticles. Ann. UMCS 2009, 64, 259-272.

20

Zhai, Y.; Dou, Y.; Liu, X.; Tu, B.; Zhao, D. Y. One-pot synthesis of magnetically separable ordered mesoporous carbon. J. Mater. Chem. 2009, 19, 3292-3300.

21

Yu, T.; Deng, Y. H.; Wang, L.; Liu, R. L.; Zhang, L. J.; Tu, B.; Zhao, D. Y. Ordered mesoporous nanocrystalline titanium-carbide/carbon composites from in situ carbothermal reduction. Adv. Mater. 2007, 19, 2301-2306.

22

Wang, H.; Wang, A. Q.; Wang, X. D.; Zhang, T. One-pot synthesized MoC imbedded in ordered mesoporous carbon as a catalyst for N2H4 decomposition. Chem. Commun. 2008, 2565-2567.

23

Zhou, J. H.; He, J. P.; Wang, T.; Sun, D.; Zhao, G. W.; Chen, X.; Wang, D. J.; Di, Z. Y. NiCl2 assisted synthesis of ordered mesoporous carbon and a new strategy for a binary catalyst. J. Mater. Chem. 2008, 18, 5776-5781.

24

Yao, J.; Li, L.; Song, H.; Liu, C.; Chen, X. Synthesis of magnetically separable ordered mesoporous carbons from F127/[Ni(H2O)6](NO3)2/resorcinol-formaldehyde composites. Carbon 2009, 47, 436-444.

25

Wang, X.; Dai, S. A simple method to ordered mesoporous carbons containing nickel nanoparticles. Adsorption 2009, 15, 138-144.

26

Ji, Z. H.; Liang, S. G.; Jiang, Y. B.; Li, H.; Liu, Z. M.; Zhao, T. Synthesis and characterization of ruthenium-containing ordered mesoporous carbon with high specific surface area. Carbon 2009, 47, 2194-2199.

27

Li, J. S.; Gu, J.; Li, H. J.; Liang, Y.; Hao, Y. X.; Sun, X. Y.; Wang, L. J. Synthesis of highly ordered Fe-containing mesoporous carbon materials using soft templating routes. Micropor. Mesopor. Mater. 2010, 128, 144-149.

28

Gao, P.; Wang, A.; Wang, X.; Zhang, T. Synthesis of highly ordered Ir-containing mesoporous carbon materials by organic-organic self-assembly. Chem. Mater. 2008, 20, 1881-1888.

29

Gao, P.; Wang, A. W.; Wang, X. D.; Zhang, T. Synthesis and catalytic performance of highly ordered Ru-containing mesoporous carbons for hydrogenation of cinnamaldehyde. Catal. Lett. 2008, 125, 289-295.

30

Liu, Q.; Wang, A.; Wang, X.; Zhang, T. Mesoporous γ-alumina synthesized by hydro-carboxylic acid as structure-directing agent. Micropor. Mesopor. Mater. 2006, 92, 10-21.

31

Yuan, Q.; Yin, A. X.; Luo, C.; Sun, L. D.; Zhang, Y. W.; Duan, W. T.; Liu, H. C.; Yan, C. H. Facile synthesis for ordered mesoporous γ-aluminas with high thermal stability. J. Am. Chem. Soc. 2008, 130, 3465-3472.

32

Meng, Y.; Gu, D.; Zhang, F. Q.; Shi, Y. F.; Yang, H. F.; Li, Z.; Yu, C. Z.; Tu, B.; Zhao, D. Y. Ordered mesoporous polymers and homologous carbon frameworks: Amphiphilic surfactant templating and direct transformation. Angew. Chem. Int. Ed. 2005, 44, 7053-7059.

33

Wan, Y.; Wang, H.; Zhao, Q.; Klingstedt, M.; Terasaki, O.; Zhao, D. Ordered mesoporous Pd/silica-carbon as a highly active heterogeneous catalyst for coupling reaction of chlorobenzene in aqueous media. J. Am. Chem. Soc. 2009, 131, 4541-4550.

File
nr-4-1-50_ESM.pdf (1.2 MB)
Publication history
Copyright
Acknowledgements
Rights and permissions

Publication history

Received: 16 July 2010
Revised: 16 August 2010
Accepted: 30 August 2010
Published: 21 October 2010
Issue date: January 2011

Copyright

© The Author(s) 2010

Acknowledgements

Acknowledgements

Support from the Natural Science Foundation of China (NSFC Nos. 20773124 and 20773122) and from the National Basic Research Program of China (No. 2009CB226102) is gratefully acknowledged. The authors thank Na Ji and Dr. Mingyuan Zheng for assistance with catalytic reactions.

Rights and permissions

This article is distributed under the terms of the Creative Commons Attribution Noncommercial License which permits any noncommercial use, distribution, and reproduction in any medium, provided the original author(s) and source are credited.

Return