Freeze-drying for controlled nanoparticle distribution in Co/SiO2 Fischer-Tropsch catalysts

被引:69
|
作者
Eggenhuisen, T. M. [1 ]
Munnik, P. [1 ]
Talsma, H. [2 ]
de Jongh, P. E. [1 ]
de Jong, K. P. [1 ]
机构
[1] Univ Utrecht, Debye Inst Nanomat Sci, NL-3584 CG Utrecht, Netherlands
[2] Univ Utrecht, Utrecht Inst Pharmaceut Sci, NL-3584 CG Utrecht, Netherlands
关键词
Nanoparticle synthesis; Lyophilization; Freeze-drying; Supported catalysts; Catalyst preparation; Fischer-Tropsch synthesis; Cobalt; Deactivation; Sintering; Transition metal nitrates; SUPPORTED CATALYSTS; CO3O4; NANOPARTICLES; COBALT CATALYSTS; NITRATE; LYOPHILIZATION; DECOMPOSITION; IMPREGNATION; TEMPERATURE; NICKEL; REDUCIBILITY;
D O I
10.1016/j.jcat.2012.10.024
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
Controlling the nanoparticle distribution over a support is considered essential to arrive at more stable catalysts. By developing a novel freeze-drying method, the nanoparticle distribution was successfully manipulated for the preparation of Co/SiO2 Fischer-Tropsch catalysts using a commercial silica-gel support. After loading the precursor via a solution impregnation or melt infiltration, differential scanning calorimetry was used to study the phase behavior of the confined cobalt nitrate precursor phases to ascertain suitable freeze-drying conditions. When a conventional drying treatment was utilized, catalysts showed inhomogeneous cobalt distributions, with 6-8 nm nanoparticles grouped in clusters of up to 400 nm. In contrast, by utilizing freeze-drying starting at liquid nitrogen temperatures, homogeneous distributions of 4-7 nm nanoparticles were obtained. Raising the temperature at which the freeze-drying process takes place resulted in either uniform or strongly non-uniform nanoparticle distributions, depending on the specific conditions and precursor loading method. After reduction, all catalysts showed high activity for the Fischer-Tropsch reaction at 1 bar. The catalysts thus synthesized form an excellent platform for future studies of the stability under industrially relevant Fischer-Tropsch conditions. (c) 2012 Elsevier Inc. All rights reserved.
引用
收藏
页码:306 / 313
页数:8
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