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

来源：

JOURNAL OF CATALYSIS | 2009年 / 262卷 / 02期

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

页码：244 / 256

页数：13

共 68 条

[51] The importance of passivation in the study of iron Fischer-Tropsch catalysts [J].

Shroff, MD ;

Datye, AK .

CATALYSIS LETTERS, 1996, 37 (1-2) :101-106

[52] ACTIVATION OF PRECIPITATED IRON FISCHER-TROPSCH SYNTHESIS CATALYSTS [J].

SHROFF, MD ;

KALAKKAD, DS ;

COULTER, KE ;

KOHLER, SD ;

HARRINGTON, MS ;

JACKSON, NB ;

SAULT, AG ;

DATYE, AK .

JOURNAL OF CATALYSIS, 1995, 156 (02) :185-207

[53]

SHULTZ JF, 1959, B US BUR MINES, V578, P50

[54]

SHULTZ JF, 1963, B US BUR MINES, V612

[55]

Storch H.H., 1951, The Fischer-Tropsch and related syntheses

[56] Formation of filamentous carbons over supported Fe catalysts through methane decomposition [J].

Takenaka, S ;

Serizawa, M ;

Otsuka, K .

JOURNAL OF CATALYSIS, 2004, 222 (02) :520-531

[57] Combining operando techniques in one spectroscopic-reaction cell:: New opportunities for elucidating the active site and related reaction mechanism in catalysis [J].

Tinnemans, SJ ;

Mesu, JG ;

Kervinen, K ;

Visser, T ;

Nijhuis, TA ;

Beale, AM ;

Keller, DE ;

van der Eerden, AMJ ;

Weckhuysen, BM .

CATALYSIS TODAY, 2006, 113 (1-2) :3-15

[58]

Vaarkamp M., 1995, PHYSICA B, V209, P159

[59] Reduction behaviour of Fe/ZrO2 and Fe/K/ZrO2 Fischer-Tropsch catalysts [J].

van den Berg, FR ;

Crajé, MWJ ;

van der Kraan, AM ;

Geus, JW .

APPLIED CATALYSIS A-GENERAL, 2003, 242 (02) :403-416

[60] Kinetics and selectivity of the Fischer-Tropsch synthesis: A literature review [J].

Van der Laan, GP ;

Beenackers, AACM .

CATALYSIS REVIEWS-SCIENCE AND ENGINEERING, 1999, 41 (3-4) :255-318

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