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Title: Improved Fischer-Tropsch synthesis catalysts for indirect coal liquefaction: Final quarterly technical progress report No. 4 for the period 1 July to 30 September 1986

Abstract

We have made significant progress in developing novel catalysts for the Fischer-Tropsch synthesis (FTS). The stoichiometries of the cluster synthesis and surface-confining reactions on an alumina support for aluminum tetra- and aluminum hexa-ruthenium hydridocarbonyl cluster catalysts were determined by gas evolution measurements. Characterization with FTIR and NMR spectroscopy of the cluster intermediates is also consistent with the observed cluster catalyst stoichiometry, Al/sub 2/O/sub 3/-Al(C/sub 2/H/sub 5/)-Ru/sub 4/H/sub 3/(CO)/sub 12/ and Al/sub 2/O/sub 3/-Al(C/sub 2/H/sub 5/)-Ru/sub 6/H(CO)/sub 18/. Activation of the surface-confined supported cluster complex by heating to 573 K in inert gas or hydrogen is likely to produce a stabilized cluster catalyst due to affinity of aluminum for alumina and the strength of the aluminum-ruthenium bonds relative to ruthenium-ligand bonds. The cluster catalysts were tested for FTS in 2:1 H/sub 2/:CO syngas at 523 K and 1 atm. The 0.6 wt % Ru/sub 4/ catalyst had superior activity and about the same selectivity through C/sub 8/ hydrocarbons as a commercial alumina-supported 0.5 wt % Ru catalyst. The 1.2 wt % Ru/sub 6/ catalyst was less active but had similar selectivity. Substantial changes in selectivity of standard-fused iron catalysts were found following treatment to uniformly chemisorb submonolayer quantities of sulfur. Approximatelymore » 40% of a monolayer of sulfur was slowly adsorbed at 473 K on the potassium-promoted fused iron catalyst following reduction and passivation by accumulation of a surface layer of carbon and CO. The passivating layer was removed and the sulfur was locally dispersed by heating to 1000 K in hydrogen. The treated catalyst had a three-fold reduction in methane selectivity-relative to untreated reduced fused iron at 573 K, and the C/sub 2/ olefin yield approached 100%. 7 refs., 1 fig., 3 tabs.« less

Authors:
; ;
Publication Date:
Research Org.:
SRI International, Menlo Park, CA (USA)
OSTI Identifier:
6956188
Report Number(s):
DOE/PC/80016-T2
ON: DE87005037
DOE Contract Number:  
AC22-85PC80016
Resource Type:
Technical Report
Resource Relation:
Other Information: Portions of this document are illegible in microfiche products
Country of Publication:
United States
Language:
English
Subject:
01 COAL, LIGNITE, AND PEAT; 10 SYNTHETIC FUELS; ALUMINIUM OXIDES; CATALYTIC EFFECTS; CATALYSTS; CHEMICAL PREPARATION; PERFORMANCE TESTING; STRUCTURAL CHEMICAL ANALYSIS; FISCHER-TROPSCH SYNTHESIS; HYDROCARBONS; SYNTHESIS; IRON; RUTHENIUM COMPLEXES; ATMOSPHERIC PRESSURE; CATALYST SUPPORTS; EXPERIMENTAL DATA; HIGH TEMPERATURE; HYDROGEN 1; INFRARED SPECTRA; NMR SPECTRA; SULFIDATION; ALUMINIUM COMPOUNDS; CHALCOGENIDES; CHEMICAL REACTIONS; COMPLEXES; DATA; ELEMENTS; HYDROGEN ISOTOPES; INFORMATION; ISOTOPES; LIGHT NUCLEI; METALS; NUCLEI; NUMERICAL DATA; ODD-EVEN NUCLEI; ORGANIC COMPOUNDS; OXIDES; OXYGEN COMPOUNDS; SPECTRA; STABLE ISOTOPES; TESTING; TRANSITION ELEMENT COMPLEXES; TRANSITION ELEMENTS; 010408* - Coal, Lignite, & Peat- C1 Processes- (1987-); 090121 - Hydrocarbon Fuels- Chemical Synthesis- (1976-1989)

Citation Formats

McCarty, J G, Wilson, R B, and Tong, G T. Improved Fischer-Tropsch synthesis catalysts for indirect coal liquefaction: Final quarterly technical progress report No. 4 for the period 1 July to 30 September 1986. United States: N. p., 1986. Web.
McCarty, J G, Wilson, R B, & Tong, G T. Improved Fischer-Tropsch synthesis catalysts for indirect coal liquefaction: Final quarterly technical progress report No. 4 for the period 1 July to 30 September 1986. United States.
McCarty, J G, Wilson, R B, and Tong, G T. Wed . "Improved Fischer-Tropsch synthesis catalysts for indirect coal liquefaction: Final quarterly technical progress report No. 4 for the period 1 July to 30 September 1986". United States.
@article{osti_6956188,
title = {Improved Fischer-Tropsch synthesis catalysts for indirect coal liquefaction: Final quarterly technical progress report No. 4 for the period 1 July to 30 September 1986},
author = {McCarty, J G and Wilson, R B and Tong, G T},
abstractNote = {We have made significant progress in developing novel catalysts for the Fischer-Tropsch synthesis (FTS). The stoichiometries of the cluster synthesis and surface-confining reactions on an alumina support for aluminum tetra- and aluminum hexa-ruthenium hydridocarbonyl cluster catalysts were determined by gas evolution measurements. Characterization with FTIR and NMR spectroscopy of the cluster intermediates is also consistent with the observed cluster catalyst stoichiometry, Al/sub 2/O/sub 3/-Al(C/sub 2/H/sub 5/)-Ru/sub 4/H/sub 3/(CO)/sub 12/ and Al/sub 2/O/sub 3/-Al(C/sub 2/H/sub 5/)-Ru/sub 6/H(CO)/sub 18/. Activation of the surface-confined supported cluster complex by heating to 573 K in inert gas or hydrogen is likely to produce a stabilized cluster catalyst due to affinity of aluminum for alumina and the strength of the aluminum-ruthenium bonds relative to ruthenium-ligand bonds. The cluster catalysts were tested for FTS in 2:1 H/sub 2/:CO syngas at 523 K and 1 atm. The 0.6 wt % Ru/sub 4/ catalyst had superior activity and about the same selectivity through C/sub 8/ hydrocarbons as a commercial alumina-supported 0.5 wt % Ru catalyst. The 1.2 wt % Ru/sub 6/ catalyst was less active but had similar selectivity. Substantial changes in selectivity of standard-fused iron catalysts were found following treatment to uniformly chemisorb submonolayer quantities of sulfur. Approximately 40% of a monolayer of sulfur was slowly adsorbed at 473 K on the potassium-promoted fused iron catalyst following reduction and passivation by accumulation of a surface layer of carbon and CO. The passivating layer was removed and the sulfur was locally dispersed by heating to 1000 K in hydrogen. The treated catalyst had a three-fold reduction in methane selectivity-relative to untreated reduced fused iron at 573 K, and the C/sub 2/ olefin yield approached 100%. 7 refs., 1 fig., 3 tabs.},
doi = {},
journal = {},
number = ,
volume = ,
place = {United States},
year = {1986},
month = {11}
}

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