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Title: Deuterium exchange and hydrogenolysis of cyclopentane as catalytic reaction probes to detect bimetallic particle formation in supported PtRe catalysts

Abstract

The H/D isotope exchange and the hydrogenolysis of cyclopentane (CP) as catalyzed by alumina or silica supported Pt, Re, the bimetallic catalyst and physical mixture, have been studied. The number of surface exposed metal atoms is determined by chemisorbing deuterium and exchanging it with hydrogen. The CP exchange reaction is found to be non-specific for the composition of the catalyzing ensembles: PtRe bimetallic catalyst exhibits the same turnover frequency (TOF) and exchange pattern as a physical mixture of these metals. The exchange rate can therefore be used to count exposed metal atoms. CP hydrogenolysis is highly ensemble-specific. The TOF for methane formation over PtRe/SiO{sub 2} exceeds that over the separate metals by a factor of 40. This finding is used to estimate the concentration of bimetallic particles in alumina supported PtRe catalysts. These reactions have also been used with temperature programmed reduction to develop a scheme by which the reduction of Re is facilitated when co-supported with Pt on {gamma}Al{sub 2}O{sub 3}. The feasibility of preparing {gamma}-Al{sub 2}O{sub 3} supported catalysts with bimetallic particles of fixed stoichiometry from the controlled deposition and decomposition of PtRe{sub 2}(CO){sub 12} was also investigated by the application of these probe reactions and FTIR. Finally,more » the effect of a chlorine on the metal function and degree of bimetallic interaction was investigated.« less

Authors:
Publication Date:
Research Org.:
Northwestern Univ., Evanston, IL (USA)
OSTI Identifier:
7203908
Resource Type:
Miscellaneous
Resource Relation:
Other Information: Thesis (Ph. D.)
Country of Publication:
United States
Language:
English
Subject:
02 PETROLEUM; 37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; CYCLOALKANES; CATALYTIC REFORMING; PLATINUM; CATALYTIC EFFECTS; RHENIUM; ALUMINIUM OXIDES; BIMETALS; CATALYST SUPPORTS; CHEMICAL PREPARATION; CHEMISORPTION; CHLORINE; DECOMPOSITION; DEHYDROGENATION; DEPOSITION; DEUTERIUM; FOURIER TRANSFORMATION; INFRARED SPECTRA; ISOTOPIC EXCHANGE; METHANE; PROMOTERS; REDUCTION; SILICON OXIDES; SURFACE PROPERTIES; SYNTHESIS; TEMPERATURE CONTROL; ALKANES; ALUMINIUM COMPOUNDS; CHALCOGENIDES; CHEMICAL REACTIONS; CONTROL; ELEMENTS; HALOGENS; HYDROCARBONS; HYDROGEN ISOTOPES; INTEGRAL TRANSFORMATIONS; ISOTOPES; LIGHT NUCLEI; METALS; NONMETALS; NUCLEI; ODD-ODD NUCLEI; ORGANIC COMPOUNDS; OXIDES; OXYGEN COMPOUNDS; PLATINUM METALS; REFORMER PROCESSES; SEPARATION PROCESSES; SILICON COMPOUNDS; SORPTION; SPECTRA; STABLE ISOTOPES; TRANSFORMATIONS; TRANSITION ELEMENTS; 020400* - Petroleum- Processing; 400201 - Chemical & Physicochemical Properties

Citation Formats

Augustine, S M. Deuterium exchange and hydrogenolysis of cyclopentane as catalytic reaction probes to detect bimetallic particle formation in supported PtRe catalysts. United States: N. p., 1988. Web.
Augustine, S M. Deuterium exchange and hydrogenolysis of cyclopentane as catalytic reaction probes to detect bimetallic particle formation in supported PtRe catalysts. United States.
Augustine, S M. 1988. "Deuterium exchange and hydrogenolysis of cyclopentane as catalytic reaction probes to detect bimetallic particle formation in supported PtRe catalysts". United States.
@article{osti_7203908,
title = {Deuterium exchange and hydrogenolysis of cyclopentane as catalytic reaction probes to detect bimetallic particle formation in supported PtRe catalysts},
author = {Augustine, S M},
abstractNote = {The H/D isotope exchange and the hydrogenolysis of cyclopentane (CP) as catalyzed by alumina or silica supported Pt, Re, the bimetallic catalyst and physical mixture, have been studied. The number of surface exposed metal atoms is determined by chemisorbing deuterium and exchanging it with hydrogen. The CP exchange reaction is found to be non-specific for the composition of the catalyzing ensembles: PtRe bimetallic catalyst exhibits the same turnover frequency (TOF) and exchange pattern as a physical mixture of these metals. The exchange rate can therefore be used to count exposed metal atoms. CP hydrogenolysis is highly ensemble-specific. The TOF for methane formation over PtRe/SiO{sub 2} exceeds that over the separate metals by a factor of 40. This finding is used to estimate the concentration of bimetallic particles in alumina supported PtRe catalysts. These reactions have also been used with temperature programmed reduction to develop a scheme by which the reduction of Re is facilitated when co-supported with Pt on {gamma}Al{sub 2}O{sub 3}. The feasibility of preparing {gamma}-Al{sub 2}O{sub 3} supported catalysts with bimetallic particles of fixed stoichiometry from the controlled deposition and decomposition of PtRe{sub 2}(CO){sub 12} was also investigated by the application of these probe reactions and FTIR. Finally, the effect of a chlorine on the metal function and degree of bimetallic interaction was investigated.},
doi = {},
url = {https://www.osti.gov/biblio/7203908}, journal = {},
number = ,
volume = ,
place = {United States},
year = {Fri Jan 01 00:00:00 EST 1988},
month = {Fri Jan 01 00:00:00 EST 1988}
}

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