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Title: Transient isotopic studies and microkinetic modeling of methane reforming over nickel catalysts

Abstract

The kinetics of elementary surface reactions involved in the reforming of methane to synthesis gas over supported nickel were studied using transient isotopic methods. To investigate methane adsorption and dehydrogenation, the reaction between CD{sub 4} and H{sub 2} was studied. To investigate water adsorption and dissociation, the reaction between H{sub 2}O and D{sub 2} was studied. To investigate the formation and cleavage of C-O bonds on the nickel surface, transient CO methanation experiments were performed. Rate constants of surface elementary reactions were extracted from the data by fitting the measured response curves to microkinetic models. An overall model that describes the reactions of methane with steam and CO{sub 2} in microkinetic terms was constructed based on these rate constants and on previously published steam reforming and CO{sub 2} methanation data. The model suggests that there is no single rate-determining step in methane reforming with either steam or CO{sub 2}, and that under some conditions the availability of surface oxygen may play a key role in determining the rate. 63 refs., 10 figs., 3 tabs.

Authors:
 [1]
  1. Haldor Topsoe Research Labs., Lyngby (Denmark)
Publication Date:
OSTI Identifier:
476810
Resource Type:
Journal Article
Journal Name:
Journal of Catalysis
Additional Journal Information:
Journal Volume: 165; Journal Issue: 2; Other Information: PBD: 15 Jan 1997
Country of Publication:
United States
Language:
English
Subject:
03 NATURAL GAS; 10 SYNTHETIC FUELS; 40 CHEMISTRY; NICKEL; CATALYTIC EFFECTS; METHANE; CATALYTIC REFORMING; CHEMICAL REACTION KINETICS; CHEMICAL PREPARATION; CATALYST SUPPORTS; DEHYDROGENATION; HETEROGENEOUS CATALYSIS; DEUTERIUM COMPOUNDS; SORPTIVE PROPERTIES; ADSORPTION

Citation Formats

Aparicio, L M. Transient isotopic studies and microkinetic modeling of methane reforming over nickel catalysts. United States: N. p., 1997. Web. doi:10.1006/jcat.1997.1468.
Aparicio, L M. Transient isotopic studies and microkinetic modeling of methane reforming over nickel catalysts. United States. doi:10.1006/jcat.1997.1468.
Aparicio, L M. Wed . "Transient isotopic studies and microkinetic modeling of methane reforming over nickel catalysts". United States. doi:10.1006/jcat.1997.1468.
@article{osti_476810,
title = {Transient isotopic studies and microkinetic modeling of methane reforming over nickel catalysts},
author = {Aparicio, L M},
abstractNote = {The kinetics of elementary surface reactions involved in the reforming of methane to synthesis gas over supported nickel were studied using transient isotopic methods. To investigate methane adsorption and dehydrogenation, the reaction between CD{sub 4} and H{sub 2} was studied. To investigate water adsorption and dissociation, the reaction between H{sub 2}O and D{sub 2} was studied. To investigate the formation and cleavage of C-O bonds on the nickel surface, transient CO methanation experiments were performed. Rate constants of surface elementary reactions were extracted from the data by fitting the measured response curves to microkinetic models. An overall model that describes the reactions of methane with steam and CO{sub 2} in microkinetic terms was constructed based on these rate constants and on previously published steam reforming and CO{sub 2} methanation data. The model suggests that there is no single rate-determining step in methane reforming with either steam or CO{sub 2}, and that under some conditions the availability of surface oxygen may play a key role in determining the rate. 63 refs., 10 figs., 3 tabs.},
doi = {10.1006/jcat.1997.1468},
journal = {Journal of Catalysis},
number = 2,
volume = 165,
place = {United States},
year = {1997},
month = {1}
}