Purified oxygen- and nitrogen-modified multi-walled carbon nanotubes as metal-free catalysts for selective olefin hydrogenation

能源化学(英文) ›› 2013, Vol. 22 ›› Issue (2): 312-320.

Purified oxygen- and nitrogen-modified multi-walled carbon nanotubes as metal-free catalysts for selective olefin hydrogenation

Peirong Chen^a, Ly May Chew^a, Aleksander Kostka^b, Kunpeng Xie^a, Martin Muhler^a, Wei Xia^a

a. Laboratory of Industrial Chemistry, Ruhr-University Bochum, 44780 Bochum, Germany;
b. Department of Microstructure Physics and Alloy Design, Max-Planck-Institute for Iron Research, 40237 Düsseldorf, Germany

收稿日期:2012-11-05 修回日期:2012-12-24 出版日期:2013-03-20 发布日期:2013-04-04
通讯作者: Wei Xia
基金资助:
This work was supported by the German Federal Ministry of Education and Research (BMBF) for the CarboKat Project (03X0204D) within the scope of the Inno.CNT Alliance.

Purified oxygen- and nitrogen-modified multi-walled carbon nanotubes as metal-free catalysts for selective olefin hydrogenation

Peirong Chen^a, Ly May Chew^a, Aleksander Kostka^b, Kunpeng Xie^a, Martin Muhler^a, Wei Xia^a

a. Laboratory of Industrial Chemistry, Ruhr-University Bochum, 44780 Bochum, Germany;
b. Department of Microstructure Physics and Alloy Design, Max-Planck-Institute for Iron Research, 40237 Düsseldorf, Germany

Received:2012-11-05 Revised:2012-12-24 Online:2013-03-20 Published:2013-04-04
Supported by:
This work was supported by the German Federal Ministry of Education and Research (BMBF) for the CarboKat Project (03X0204D) within the scope of the Inno.CNT Alliance.

摘要/Abstract

摘要： Oxygen- and nitrogen-functionalized carbon nanotubes (OCNTs and NCNTs) were applied as metal-free catalysts in selective olefin hydrogenation. A series of NCNTs was synthesized by NH₃ post-treatment of OCNTs. Temperature-programmed desorption, N₂ physisorption, Raman spectroscopy, high-resolution transmission electron microscopy and X-ray photoelectron spectroscopy were employed to characterize the surface properties of OCNTs and NCNTs, aiming at a detailed analysis of the type and amount of oxygen- and nitrogen-containing groups as well as surface defects. The gas-phase treatments applied for oxygen and nitrogen functionalization at elevated temperatures up to 600 ℃ led to the increase of surface defects, but did not cause structural damages in the bulk. NCNTs showed a clearly higher activity than the pristine CNTs and OCNTs in the hydrogenation of 1,5-cyclooctadiene, and also the selectivity to cyclooctene was higher. The favorable catalytic properties are ascribed to the nitrogen-containing surface functional groups as well as surface defects related to nitrogen species. In contrast, oxygen-containing surface groups and the surface defects caused by oxygen species did not show clear contribution to the hydrogenation catalysis.

关键词: multi-walled carbon nanotubes, nitrogen-containing functional groups, oxygen-containing functional groups, metal-free catalyst, selective olefin hydrogenation

Abstract: Oxygen- and nitrogen-functionalized carbon nanotubes (OCNTs and NCNTs) were applied as metal-free catalysts in selective olefin hydrogenation. A series of NCNTs was synthesized by NH₃ post-treatment of OCNTs. Temperature-programmed desorption, N₂ physisorption, Raman spectroscopy, high-resolution transmission electron microscopy and X-ray photoelectron spectroscopy were employed to characterize the surface properties of OCNTs and NCNTs, aiming at a detailed analysis of the type and amount of oxygen- and nitrogen-containing groups as well as surface defects. The gas-phase treatments applied for oxygen and nitrogen functionalization at elevated temperatures up to 600 ℃ led to the increase of surface defects, but did not cause structural damages in the bulk. NCNTs showed a clearly higher activity than the pristine CNTs and OCNTs in the hydrogenation of 1,5-cyclooctadiene, and also the selectivity to cyclooctene was higher. The favorable catalytic properties are ascribed to the nitrogen-containing surface functional groups as well as surface defects related to nitrogen species. In contrast, oxygen-containing surface groups and the surface defects caused by oxygen species did not show clear contribution to the hydrogenation catalysis.

Key words: multi-walled carbon nanotubes, nitrogen-containing functional groups, oxygen-containing functional groups, metal-free catalyst, selective olefin hydrogenation

Peirong Chen, Ly May Chew, Aleksander Kostka, Kunpeng Xie, Martin Muhler, Wei Xia. Purified oxygen- and nitrogen-modified multi-walled carbon nanotubes as metal-free catalysts for selective olefin hydrogenation[J]. 能源化学(英文), 2013, 22(2): 312-320.

参考文献

[1] Gong K P, Du F, Xia Z H, Durstock M, Dai L M. Science, 2009, 323(5915): 760
[2] Yu H, Peng F, Tan J, Hu X W, Wang H J, Yang J A, Zheng W X. Angew Chem Int Ed, 2011, 50(17): 3978
[3] Kundu S, Xia W, Busser W, Becker M, Schmidt D A, Havenith M, Muhler M. Phys Chem Chem Phys, 2010, 12(17): 4351
[4] Chizari K, Deneuve A, Ersen O, Florea I, Liu Y, Edouard D, Janowska I, Begin D, Pham-Huu C. ChemSusChem, 2012, 5(1): 102
[5] Hu X B, Wu Y J, Li H R, Zhang Z B. J Phys Chem C, 2010, 114(21): 9603
[6] Kundu S, Nagaiah T C, Xia W, Wang Y M, Van Dommele S, Bitter J H, Santa M, Grundmeier G, Bron M, Schuhmann W, Muhler M. J Phys Chem C, 2009, 113(32): 14302
[7] Jin C, Nagaiah T C, Xia W, Spliethoff B, Wang S S, Bron M, Schuhmann W, Muhler M. Nanoscale, 2010, 2(6): 981
[8] Nagaiah T C, Kundu S, Bron M, Muhler M, Schuhmann W. Electrochem Commun, 2010, 12(3): 338
[9] Wang Z J, Jia R R, Zheng J F, Zhao J G, Li L, Song J L, Zhu Z P. ACS Nano, 2011, 5(3): 1677
[10] Yu D S, Zhang Q, Dai L M. J Am Chem Soc, 2010, 132(43): 15127
[11] Banks C E, Crossley A, Salter C, Wilkins S J, Compton R G. Angew Chem Int Ed, 2006, 45(16): 2533
[12] Wiggins-Camacho J D. Stevenson K J. J Phys Chem C, 2011, 115(40): 20002
[13] Florea I, Ersen O, Arenal R, Ihiawakrim D, Messaoudi C, Chizari K, Janowska I, Pham-Huu C. J Am Chem Soc, 2012, 134(23): 9672
[14] Hu X B, Zhou Z, Lin Q X, Wu Y J, Zhang Z B. Chem Phys Lett, 2011, 503(4-6): 287
[15] Sankaran M, Viswanathan B. Carbon, 2006, 44(13): 2816
[16] Zhang Z Y, Cho K. Phys Rev B, 2007, 75(7): 075420
[17] Su D S, Zhang J, Frank B, Thomas A, Wang X C, Paraknowitsch J, Schlögl R. ChemSusChem, 2010, 3(2): 169
[18] Xia W, Jin C, Kundu S, Muhler M. Carbon, 2009, 47(3): 919
[19] Schmidt A, Schomäcker R. Ind Eng Chem Res, 2007, 46(6): 1677
[20] Jin C, Xia W, Chen P R, Muhler M. Catal Today, 2012, 186(1): 128
[21] Li C, Zhao A Q, Xia W, Liang C H, Muhler M. J. Phys Chem C, 2012, 116(39): 20930
[22] Kundu S, Wang Y M, Xia W, Muhler M. J Phys Chem C, 2008, 112(43): 16869
[23] Xia W, Yin X L, Kundu S, Sanchez M, Birkner A, Wöll C, Muhler M. Carbon, 2011, 49(1): 299

Purified oxygen- and nitrogen-modified multi-walled carbon nanotubes as metal-free catalysts for selective olefin hydrogenation

Purified oxygen- and nitrogen-modified multi-walled carbon nanotubes as metal-free catalysts for selective olefin hydrogenation

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