Local and long range order in promoted iron-based Fischer-Tropsch catalysts: A combined in situ X-ray absorption spectroscopy/wide angle X-ray

被引:159
作者
de Smit, Emiel [1 ]
Beale, Andrew M. [1 ]
Nikitenko, Sergey [2 ]
Weckhuysen, Bert M. [1 ]
机构
[1] Univ Utrecht, Debye Inst Nanomat Sci, NL-3584 CA Utrecht, Netherlands
[2] European Synchrotron Radiat Facil, DUBBLE, Netherlands Org Sci Res NWO, F-38043 Grenoble 9, France
关键词
Fischer-Tropsch synthesis; Iron; Catalyst promotion; In situ; XAFS; WAXS; SUPPORTED FE CATALYSTS; MOSSBAUER-SPECTROSCOPY; REDUCTION BEHAVIOR; WORKING CATALYST; ANOMALOUS WATER; ACTIVATION; CARBON; CARBIDE; SILICA; DIFFRACTION;
D O I
10.1016/j.jcat.2008.12.021
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
The structural properties of three Fe-based Fischer-Tropsch synthesis (FTS) catalysts containing different amounts of Cu, K and SiO2 additives were investigated during pretreatment and FTS in a fixed bed-like reactor using combined in situ X-ray absorption fine structure (XAFS)/wide angle X-ray scattering (WARS) techniques. This combination enabled acquisition of complementary information regarding the local environment of iron atoms from XAFS and crystalline phases from WAXS during H-2 and CO/H-2 pretreatment and FTS at 1 bar. The presence of the SiO2 support and promoter elements significantly influenced the structural properties of the catalysts after pretreatment. After FTS, H-2 pretreated catalysts mainly consisted of amorphous theta-Fe3C clusters (unsupported catalysts) or amorphous iron (II) silicate (supported catalyst), while the CO/H-2 pretreated catalysts all consisted mainly of gamma-Fe and chi-Fe5C2. Catalysts activated in CO/H-2 showed superior stability and activity, while H-2 pretreated unsupported catalysts deactivated rapidly during the first 15 h of FTS. (C) 2009 Elsevier Inc. All rights reserved.
引用
收藏
页码:244 / 256
页数:13
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