The Molecular Mechanism of Low-Temperature Decomposition of Hydrogen Sulfide under Conjugated Chemisorption–Catalysis Conditions Full article
Journal |
Russian Journal of Physical Chemistry A
ISSN: 0036-0244 , E-ISSN: 1531-863X |
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Output data | Year: 2006, Volume: 80, Number: 9, Pages: 1403-1410 Pages count : 8 DOI: 10.1134/S0036024406090081 | ||
Tags | Hydrogen Molecule; Density Functional Theory Method; Surface Intermediate; Dissociative Chemisorption; Balance Energy Expenditure | ||
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Affiliations |
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Funding (1)
1 | Russian Foundation for Basic Research | 04-03-32188 |
Abstract:
The molecular mechanism of interaction of two hydrogen sulfide molecules with the (CoIII-Ho)2S2(SH2)4 model active center containing occluded hydrogen was studied by the density functional theory method with the B3P86 hybrid exchange-correlation functional. The reaction was found to occur in the following elementary steps: molecular adsorption of hydrogen sulfide ⇒ dissociative chemisorption ⇒ S-S bond formation in the surface intermediate {2CoIII − (μ-S2) + 2H(ads)} with the release of the first hydrogen molecule into the gas phase H2(g) ⇒ the release of the second hydrogen molecule into the gas phase H2(g) ⇒ the formation of cyclooctasulfur in the reaction 4S2(ads) → S8(ads). The first three steps occur spontaneously at room temperature, the thermodynamic driving force of the process being the stoichiometric reaction of S-S bond formation at the stage of conjugated chemisorption of two hydrogen sulfide molecules on two adjacent metal ions with the release of the first hydrogen molecule into the gas phase. The catalytic cycle is terminated by the recombination of molecular sulfur S2 into cyclooctasulfur S8 in the adsorption layer and the release of the second hydrogen molecule into the gas phase.
Cite:
Zakharov I.I.
, Startsev A.N.
, Voroshina O.V.
, Pashigreva A.V.
, Chashkova N.A.
, Parmon V.N.
The Molecular Mechanism of Low-Temperature Decomposition of Hydrogen Sulfide under Conjugated Chemisorption–Catalysis Conditions
Russian Journal of Physical Chemistry A. 2006. V.80. N9. P.1403-1410. DOI: 10.1134/S0036024406090081 WOS Scopus РИНЦ
The Molecular Mechanism of Low-Temperature Decomposition of Hydrogen Sulfide under Conjugated Chemisorption–Catalysis Conditions
Russian Journal of Physical Chemistry A. 2006. V.80. N9. P.1403-1410. DOI: 10.1134/S0036024406090081 WOS Scopus РИНЦ
Original:
Захаров И.И.
, Старцев А.Н.
, Ворошина О.В.
, Пашигрева А.В.
, Чашкова Н.А.
, Пармон В.Н.
Молекулярный механизм низкотемпературного разложения сероводорода в условиях сочетания сопряженной хемосорбции и катализа
Журнал физической химии. 2006. Т.80. №9. С.1589-1596. RSCI РИНЦ
Молекулярный механизм низкотемпературного разложения сероводорода в условиях сочетания сопряженной хемосорбции и катализа
Журнал физической химии. 2006. Т.80. №9. С.1589-1596. RSCI РИНЦ
Dates:
Submitted: | Sep 2, 2005 |
Published print: | Sep 1, 2006 |
Identifiers:
Web of science | WOS:000245666700008 |
Scopus | 2-s2.0-33750147828 |
Elibrary | 13526901 |
Chemical Abstracts | 2006:898259 |
Chemical Abstracts (print) | 145:276817 |
OpenAlex | W1997233498 |