Nitrogen-Doped Carbon Nanotubes as a Highly Active Metal-Free Catalyst for Selective Oxidation

被引:171
作者
Chizari, Kambiz [1 ]
Deneuve, Adrien [1 ]
Ersen, Ovidiu [2 ]
Florea, Ileana [2 ]
Liu, Yu [1 ]
Edouard, David [1 ]
Janowska, Izabela [1 ]
Begin, Dominique [1 ]
Cuong Pham-Huu [1 ]
机构
[1] Univ Strasbourg, LMSPC, CNRS, UMR 7515, F-67087 Strasbourg 02, France
[2] Univ Strasbourg, IPCMS, CNRS, UMR 7504, F-67037 Strasbourg 08, France
关键词
heterogeneous catalysis; macroscopic shaping; nanotubes; oxidation; sulfur; HYDROGEN-SULFIDE; ELEMENTAL SULFUR; OXIDE CATALYSTS; SURFACE-CHEMISTRY; OXYGEN REDUCTION; MIXED-OXIDE; H2S; ADSORPTION; IRON; NANOMATERIALS;
D O I
10.1002/cssc.201100276
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Catalytic reactions are generally carried out on supported metals or oxides, which act as an active phase and require impregnation and thermal treatment steps. During tests, the metal or oxide nanoparticles could be further sintered, which would induces deactivation. Direct incorporation of the active phase into the matrix of a support could be an elegant alternative to prevent catalyst deactivation. Here, we report that nitrogen-doped carbon nanotubes (N-CNTs) can be efficiently employed as a metal-free catalyst for oxidative reactions that allow the selective transformation of the harmful, gaseous H2S into solid sulfur. The catalyst exhibits a high stability during the test at high space velocity. The macroscopic shaping of the catalyst on the silicon carbide foam also increases its catalytic activity by improving the contact between the reactants and the catalyst. Such macroscopic shaping allows the avoidance of problems linked with transport and handling of nanoscopic materials and also reduces the pressure drop across the catalyst bed to a large extent.
引用
收藏
页码:102 / 108
页数:7
相关论文
共 44 条
[1]   Analysis of the relationship between H2S removal capacity and surface properties of unimpregnated activated carbons [J].
Adib, F ;
Bagreev, A ;
Bandosz, TJ .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2000, 34 (04) :686-692
[2]   N-doped carbon nanotubes for liquid-phase C=C bond hydrogenation [J].
Amadou, Julien ;
Chizari, Kambiz ;
Houlle, Matthieu ;
Janowska, Izabela ;
Ersen, Ovidiu ;
Begin, Dominique ;
Pham-Huu, Cuong .
CATALYSIS TODAY, 2008, 138 (1-2) :62-68
[3]   H2S adsorption/oxidation on unmodified activated carbons:: importance of prehumidification [J].
Bagreev, A ;
Bandosz, TJ .
CARBON, 2001, 39 (15) :2303-2311
[4]   Carbon nanotubes - the route toward applications [J].
Baughman, RH ;
Zakhidov, AA ;
de Heer, WA .
SCIENCE, 2002, 297 (5582) :787-792
[5]   Oxidative dehydrogenation of 9,10-dihydroanthracene using multi-walled carbon nanotubes [J].
Begin, Dominique ;
Ulrich, Gilles ;
Amadou, Julien ;
Su, Dang Sheng ;
Pham-Huu, Cuong ;
Ziessel, Raymond .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 2009, 302 (1-2) :119-123
[6]   The characterization of activated carbons with oxygen and nitrogen surface groups [J].
Biniak, S ;
Szymanski, G ;
Siedlewski, J ;
Swiatkowski, A .
CARBON, 1997, 35 (12) :1799-1810
[7]   PtRu nanoparticles supported on nitrogen-doped multiwalled carbon nanotubes as catalyst for methanol electrooxidation [J].
Chetty, Raghuram ;
Kundu, Shankhamala ;
Xia, Wei ;
Bron, Michael ;
Schuhmann, Wolfgang ;
Chirila, Valentin ;
Brandl, Waltraut ;
Reinecke, Thomas ;
Muhler, Martin .
ELECTROCHIMICA ACTA, 2009, 54 (17) :4208-4215
[8]   Tuning of nitrogen-doped carbon nanotubes as catalyst support for liquid-phase reaction [J].
Chizari, Kambiz ;
Janowska, Izabela ;
Houlle, Matthieu ;
Florea, Ileana ;
Ersen, Ovidiu ;
Romero, Thierry ;
Bernhardt, Pierre ;
Ledoux, Marc Jacques ;
Pham-Huu, Cuong .
APPLIED CATALYSIS A-GENERAL, 2010, 380 (1-2) :72-80
[9]   Distribution and structure of N atoms in multiwalled carbon nanotubes using variable-energy X-ray photoelectron spectroscopy [J].
Choi, HC ;
Park, J ;
Kim, B .
JOURNAL OF PHYSICAL CHEMISTRY B, 2005, 109 (10) :4333-4340
[10]   Experimental and theoretical studies on the structure of N-doped carbon nanotubes:: Possibility of intercalated molecular N2 [J].
Choi, HC ;
Bae, SY ;
Park, J ;
Seo, K ;
Kim, C ;
Kim, B ;
Song, HJ ;
Shin, HJ .
APPLIED PHYSICS LETTERS, 2004, 85 (23) :5742-5744