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Title: Preparation and EXAFS studies of highly dispersed iron catalyst derived from Fe[sub 3](CO)[sub 12] precipitated on alumina

Abstract

Supported tri-iron dodecacarbonyl has been prepared by a novel method, precipitating the cluster on alumina without any pretreatment. The precipitated Fe[sub 3](CO)[sub 12]/Al[sub 2]O[sub 3] retains a molecular structure similar to that of its parent compound as demonstrated by Fe K-edge XANES (X-ray adsorption near-edge structure) and infrared results. After decarbonylation under very mild conditions (310 K in vacuum), the Fe/Al[sub 2]O[sub 3] obtained exhibits a good catalytic selectivity for lower olefins in the hydrogenation of carbon monoxide. K-edge EXAFS (extended X-ray adsorption fine structure) analyses of the fresh catalyst and the used catalyst suggest that the active site on the surface is an ensemble of three iron atoms with one short Fe-Fe bond of 2.52 [plus minus] 0.05 [angstrom] and two longer Fe-Fe bonds of 2.74 [plus minus] 0.04 [angstrom]. However, the aggregation of these Fe[sub 3] groups to particles over 10 [angstrom] in size brings about a short lifetime and poor selectivity for the catalyst. The aggregated particles are still two-dimensional, consisting of at least three iron trimers in which the interatomic distance for each trimer of iron on the average is 2.48 [plus minus] 0.08 [angstrom], and the nearest interatomic distance between two trimers is 2.83 [plusmore » minus] 0.03 [angstrom]. 26 refs., 7 figs., 3 tabs.« less

Authors:
; ;  [1];  [2];  [3]
  1. Lanzhou Institute of Chemical Physics (China)
  2. Kyoto Univ. (Japan)
  3. Photon Factory, Tsukuba (Japan)
Publication Date:
OSTI Identifier:
5989975
Resource Type:
Journal Article
Journal Name:
Journal of Catalysis; (United States)
Additional Journal Information:
Journal Volume: 141:2; Journal ID: ISSN 0021-9517
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; 01 COAL, LIGNITE, AND PEAT; ALUMINIUM OXIDES; STRUCTURAL CHEMICAL ANALYSIS; CARBON MONOXIDE; HYDROGENATION; IRON; ABSORPTION SPECTROSCOPY; ALKENES; CATALYST SUPPORTS; CATALYSTS; CATALYTIC EFFECTS; CHEMICAL PREPARATION; FINE STRUCTURE; HETEROGENEOUS CATALYSIS; X-RAY SPECTROSCOPY; ALUMINIUM COMPOUNDS; CARBON COMPOUNDS; CARBON OXIDES; CATALYSIS; CHALCOGENIDES; CHEMICAL REACTIONS; ELEMENTS; HYDROCARBONS; METALS; ORGANIC COMPOUNDS; OXIDES; OXYGEN COMPOUNDS; SPECTROSCOPY; SYNTHESIS; TRANSITION ELEMENTS; 400201* - Chemical & Physicochemical Properties; 010408 - Coal, Lignite, & Peat- C1 Processes- (1987-)

Citation Formats

Kou, Y, Wang, H L, Te, M, Tanaka, Tsunehiro, and Nomura, Masaharu. Preparation and EXAFS studies of highly dispersed iron catalyst derived from Fe[sub 3](CO)[sub 12] precipitated on alumina. United States: N. p., 1993. Web. doi:10.1006/jcat.1993.1171.
Kou, Y, Wang, H L, Te, M, Tanaka, Tsunehiro, & Nomura, Masaharu. Preparation and EXAFS studies of highly dispersed iron catalyst derived from Fe[sub 3](CO)[sub 12] precipitated on alumina. United States. https://doi.org/10.1006/jcat.1993.1171
Kou, Y, Wang, H L, Te, M, Tanaka, Tsunehiro, and Nomura, Masaharu. Tue . "Preparation and EXAFS studies of highly dispersed iron catalyst derived from Fe[sub 3](CO)[sub 12] precipitated on alumina". United States. https://doi.org/10.1006/jcat.1993.1171.
@article{osti_5989975,
title = {Preparation and EXAFS studies of highly dispersed iron catalyst derived from Fe[sub 3](CO)[sub 12] precipitated on alumina},
author = {Kou, Y and Wang, H L and Te, M and Tanaka, Tsunehiro and Nomura, Masaharu},
abstractNote = {Supported tri-iron dodecacarbonyl has been prepared by a novel method, precipitating the cluster on alumina without any pretreatment. The precipitated Fe[sub 3](CO)[sub 12]/Al[sub 2]O[sub 3] retains a molecular structure similar to that of its parent compound as demonstrated by Fe K-edge XANES (X-ray adsorption near-edge structure) and infrared results. After decarbonylation under very mild conditions (310 K in vacuum), the Fe/Al[sub 2]O[sub 3] obtained exhibits a good catalytic selectivity for lower olefins in the hydrogenation of carbon monoxide. K-edge EXAFS (extended X-ray adsorption fine structure) analyses of the fresh catalyst and the used catalyst suggest that the active site on the surface is an ensemble of three iron atoms with one short Fe-Fe bond of 2.52 [plus minus] 0.05 [angstrom] and two longer Fe-Fe bonds of 2.74 [plus minus] 0.04 [angstrom]. However, the aggregation of these Fe[sub 3] groups to particles over 10 [angstrom] in size brings about a short lifetime and poor selectivity for the catalyst. The aggregated particles are still two-dimensional, consisting of at least three iron trimers in which the interatomic distance for each trimer of iron on the average is 2.48 [plus minus] 0.08 [angstrom], and the nearest interatomic distance between two trimers is 2.83 [plus minus] 0.03 [angstrom]. 26 refs., 7 figs., 3 tabs.},
doi = {10.1006/jcat.1993.1171},
url = {https://www.osti.gov/biblio/5989975}, journal = {Journal of Catalysis; (United States)},
issn = {0021-9517},
number = ,
volume = 141:2,
place = {United States},
year = {1993},
month = {6}
}