Effect of support surface treatment on the synthesis, structure, and performance of Co/CNT Fischer-Tropsch catalysts

被引:83
作者
Eschemann, Thomas O. [1 ]
Lamme, Wouter S. [1 ]
Manchester, Rene L. [1 ]
Parmentier, Tanja E. [1 ,2 ]
Cognigni, Andrea [2 ]
Ronning, Magnus [2 ]
de Jong, Krijn P. [1 ]
机构
[1] Univ Utrecht, Debye Inst Nanomat Sci, Inorgan Chem & Catalysis, NL-3508 TB Utrecht, Netherlands
[2] Norwegian Univ Sci & Technol NTNU, Dept Chem Engn, NO-7491 Trondheim, Norway
关键词
Fischer-Tropsch; Carbon nanotubes (CNT); Cobalt; Impregnation; Solvent effects; Surface functionalization; Gas-phase oxidation; COBALT PARTICLE-SIZE; HIGH-RESOLUTION XPS; CARBON NANOTUBES; HYDROCARBON SELECTIVITY; PRODUCT DISTRIBUTION; NOBLE-METALS; FIXED-BED; OXYGEN; NANOFIBERS; RAMAN;
D O I
10.1016/j.jcat.2014.12.010
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
We report the preparation of supported cobalt catalysts (9 wt% Co) on untreated (CNT) and surface-oxidized (CNT-ox) carbon nanotube materials by incipient wetness impregnation with solutions of cobalt nitrate in water, ethanol, or 1-propanol. The results show that by a judicious selection of solvent and drying method, similar cobalt oxide particle sizes in the range of 4-5 nm on CNT and CNT-ox materials were obtained for the fresh catalysts. Cobalt particles supported on unfunctionalized CNT showed higher initial activities and C5+-selectivities than catalysts on functionalized CNT; however, the former catalysts were more prone to cobalt particle growth due to the lack of anchoring sites. The activities and cobalt particle sizes of catalysts after 60 h on stream revealed for particles larger than 6 nm a turnover frequencies (TOF) of 0.07 s(-1) for Co/CNT and 0.03 s(-1) for Co/CNT-ox. In situ XAS/XRPD studies showed a similar degree of reduction for the catalysts on untreated and oxidized CNT and the formation of hcp cobalt metal on untreated CNT which rationalizes the higher activity and TOF of the Co/CNT catalysts. (C) 2014 Elsevier Inc. All rights reserved.
引用
收藏
页码:130 / 138
页数:9
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