Carbon nanotubes decorated α-Al2O3 containing cobalt nanoparticles for Fischer-Tropsch reaction

能源化学(英文) ›› 2013, Vol. 22 ›› Issue (2): 279-289.

Carbon nanotubes decorated α-Al₂O₃ containing cobalt nanoparticles for Fischer-Tropsch reaction

Yuefeng Liu^a, Thierry Dintzer^a, Ovidiu Ersen^b, Cuong Pham-Huu^a

a. Laboratoire des Matériaux, Surfaces et Procédés pour la Catalyse (LMSPC), UMR 7515 CNRS-Université de Strasbourg (UdS), 25, rue Becquerel, 67087 Strasbourg Cedex 08, France;
b. Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), UMR 7504 CNRS-Université de Strasbourg (UdS), 23, rue du Loess, 67037 Strasbourg Cedex 02, France

收稿日期:2012-10-26 修回日期:2012-12-14 出版日期:2013-03-20 发布日期:2013-04-04
通讯作者: Yuefeng Liu, Cuong Pham-Huu
基金资助:
Y. F. Liu would like to thank the China Scholarship Council (CSC) for the PhD grant during his stay at the LMSPC. SEM and TEM experiments were carried out at the facilities of IPCMS (UMR 7504 CNRS). Fabrice Vigneron, Thierry Romero, Walid Baaziz and Jingjie Luo (LMSPC) are gratefully acknowledged for discussion and experimental assistance.

Carbon nanotubes decorated α-Al₂O₃ containing cobalt nanoparticles for Fischer-Tropsch reaction

Yuefeng Liu^a, Thierry Dintzer^a, Ovidiu Ersen^b, Cuong Pham-Huu^a

a. Laboratoire des Matériaux, Surfaces et Procédés pour la Catalyse (LMSPC), UMR 7515 CNRS-Université de Strasbourg (UdS), 25, rue Becquerel, 67087 Strasbourg Cedex 08, France;
b. Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), UMR 7504 CNRS-Université de Strasbourg (UdS), 23, rue du Loess, 67037 Strasbourg Cedex 02, France

Received:2012-10-26 Revised:2012-12-14 Online:2013-03-20 Published:2013-04-04
Supported by:
Y. F. Liu would like to thank the China Scholarship Council (CSC) for the PhD grant during his stay at the LMSPC. SEM and TEM experiments were carried out at the facilities of IPCMS (UMR 7504 CNRS). Fabrice Vigneron, Thierry Romero, Walid Baaziz and Jingjie Luo (LMSPC) are gratefully acknowledged for discussion and experimental assistance.

摘要/Abstract

摘要： A new hierarchical composite consisted of multi-walled carbon nanotubes (CNTs) layer anchored on macroscopic α-Al₂O₃ host matrix was synthesized and used as support for Fischer-Tropsch synthesis (FTS). The composite constituted by a thin shell of a homogeneous, highly entangled and structure-opened carbon nanotubes network and it exhibited a relatively high and fully accessible specific surface area of 76 m²·g^-1, compared with that of 5 m²·g^-1 of the original α-Al₂O₃support. The metal-support interaction between carbon nanotubes surface and cobalt precursor and high effective surface area led to a relatively high dispersion of cobalt nanoparticles. This hierarchically supported cobalt catalyst exhibited a high FTS activity along with an extremely high selectivity towards liquid hydrocarbons compared with the cobalt-based catalyst supported on pristine α-Al₂O₃ or on CNTs carriers. This improvement can attribute to the high accessibility of composite surface area comparing with the macroscopic host structure alone or to the bulk CNTs where the nanoscopic dimension induced a dense packing with low mass transfer which favoured the problem of reactants competitive diffusion towards the cobalt active site. In addition, intrinsic thermal conductivity of decorated CNTs could help the heat dissipating throughout the catalyst body, thus avoiding the formation of local hot spots which appeared in high CO conversion under pure syngas feed in FTS reaction. Cobalt supported on CNTs decorated α-Al₂O₃ catalyst also exhibited satisfied high stability during more than 200 h on stream under relatively severe conditions compared with other catalysts reported in the literature. Finally, the macroscopic shape of such composite easily rendered its usage as catalyst support in a fixed-bed configuration without facing problems of transport and pressure drop as encountered with the bulk CNTs.

关键词: carbon nanotubes, Fischer-Tropsch synthesis, α-Al₂O₃, hierarchical support, cobalt nanoparticles

Abstract: A new hierarchical composite consisted of multi-walled carbon nanotubes (CNTs) layer anchored on macroscopic α-Al₂O₃ host matrix was synthesized and used as support for Fischer-Tropsch synthesis (FTS). The composite constituted by a thin shell of a homogeneous, highly entangled and structure-opened carbon nanotubes network and it exhibited a relatively high and fully accessible specific surface area of 76 m²·g^-1, compared with that of 5 m²·g^-1 of the original α-Al₂O₃support. The metal-support interaction between carbon nanotubes surface and cobalt precursor and high effective surface area led to a relatively high dispersion of cobalt nanoparticles. This hierarchically supported cobalt catalyst exhibited a high FTS activity along with an extremely high selectivity towards liquid hydrocarbons compared with the cobalt-based catalyst supported on pristine α-Al₂O₃ or on CNTs carriers. This improvement can attribute to the high accessibility of composite surface area comparing with the macroscopic host structure alone or to the bulk CNTs where the nanoscopic dimension induced a dense packing with low mass transfer which favoured the problem of reactants competitive diffusion towards the cobalt active site. In addition, intrinsic thermal conductivity of decorated CNTs could help the heat dissipating throughout the catalyst body, thus avoiding the formation of local hot spots which appeared in high CO conversion under pure syngas feed in FTS reaction. Cobalt supported on CNTs decorated α-Al₂O₃ catalyst also exhibited satisfied high stability during more than 200 h on stream under relatively severe conditions compared with other catalysts reported in the literature. Finally, the macroscopic shape of such composite easily rendered its usage as catalyst support in a fixed-bed configuration without facing problems of transport and pressure drop as encountered with the bulk CNTs.

Key words: carbon nanotubes, Fischer-Tropsch synthesis, α-Al₂O₃, hierarchical support, cobalt nanoparticles

Yuefeng Liu, Thierry Dintzer, Ovidiu Ersen, Cuong Pham-Huu. Carbon nanotubes decorated α-Al₂O₃ containing cobalt nanoparticles for Fischer-Tropsch reaction[J]. 能源化学(英文), 2013, 22(2): 279-289.

Yuefeng Liu, Thierry Dintzer, Ovidiu Ersen, Cuong Pham-Huu. Carbon nanotubes decorated α-Al₂O₃ containing cobalt nanoparticles for Fischer-Tropsch reaction[J]. Journal of Energy Chemistry, 2013, 22(2): 279-289.

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Carbon nanotubes decorated α-Al₂O₃ containing cobalt nanoparticles for Fischer-Tropsch reaction

Carbon nanotubes decorated α-Al₂O₃ containing cobalt nanoparticles for Fischer-Tropsch reaction

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