The mechanism of the catalytic oxidation of hydrogen sulfide *1: III. An electron spin resonance study of the sulfur catalyzed oxidation of hydrogen sulfide

M. Steijns, P. Koopman, B. Nieuwenhuijse, P. Mars

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Abstract

ESR experiments on the oxidation of hydrogen sulfide were performed in the temperature range 20–150 °C. Alumina, active carbon and molecular sieve zeolite 13X were investigated as catalysts. For zeolite 13X it was demonstrated that the reaction is autocatalytic and that sulfur radicals are the active sites for oxygen chemisorption. The intensity of the sulfur radical ESR signal, which is related to the degree of conversion of these radicals, by oxygen, fits in with an oxidation-reduction mechanism. The sulfur-oxygen radical species, which appear when oxygen is admitted to sulfur radicals, are assigned to sulfur chains containing one or two oxygen atoms at the end of the chain. It is very likely that these sulfur-oxygen radicals are intermediates in the proposed mechanism. The formation of the byproduct SO2 from SxO2 · − at temperatures above 175 °C is also visible in the ESR spectrum. On the basis of the experiments it is concluded that in the mechanism of H2S oxidation on active carbons, carbon radicals do not play an important role.
Original languageUndefined
Pages (from-to)96-106
JournalJournal of catalysis
Volume42
Issue number1
DOIs
Publication statusPublished - 1976

Keywords

  • IR-68342

Cite this

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title = "The mechanism of the catalytic oxidation of hydrogen sulfide *1: III. An electron spin resonance study of the sulfur catalyzed oxidation of hydrogen sulfide",
abstract = "ESR experiments on the oxidation of hydrogen sulfide were performed in the temperature range 20–150 °C. Alumina, active carbon and molecular sieve zeolite 13X were investigated as catalysts. For zeolite 13X it was demonstrated that the reaction is autocatalytic and that sulfur radicals are the active sites for oxygen chemisorption. The intensity of the sulfur radical ESR signal, which is related to the degree of conversion of these radicals, by oxygen, fits in with an oxidation-reduction mechanism. The sulfur-oxygen radical species, which appear when oxygen is admitted to sulfur radicals, are assigned to sulfur chains containing one or two oxygen atoms at the end of the chain. It is very likely that these sulfur-oxygen radicals are intermediates in the proposed mechanism. The formation of the byproduct SO2 from SxO2 · − at temperatures above 175 °C is also visible in the ESR spectrum. On the basis of the experiments it is concluded that in the mechanism of H2S oxidation on active carbons, carbon radicals do not play an important role.",
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year = "1976",
doi = "10.1016/0021-9517(76)90095-6",
language = "Undefined",
volume = "42",
pages = "96--106",
journal = "Journal of catalysis",
issn = "0021-9517",
publisher = "Academic Press Inc.",
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The mechanism of the catalytic oxidation of hydrogen sulfide *1: III. An electron spin resonance study of the sulfur catalyzed oxidation of hydrogen sulfide. / Steijns, M.; Koopman, P.; Nieuwenhuijse, B.; Mars, P.

In: Journal of catalysis, Vol. 42, No. 1, 1976, p. 96-106.

Research output: Contribution to journalArticleAcademic

TY - JOUR

T1 - The mechanism of the catalytic oxidation of hydrogen sulfide *1: III. An electron spin resonance study of the sulfur catalyzed oxidation of hydrogen sulfide

AU - Steijns, M.

AU - Koopman, P.

AU - Nieuwenhuijse, B.

AU - Mars, P.

PY - 1976

Y1 - 1976

N2 - ESR experiments on the oxidation of hydrogen sulfide were performed in the temperature range 20–150 °C. Alumina, active carbon and molecular sieve zeolite 13X were investigated as catalysts. For zeolite 13X it was demonstrated that the reaction is autocatalytic and that sulfur radicals are the active sites for oxygen chemisorption. The intensity of the sulfur radical ESR signal, which is related to the degree of conversion of these radicals, by oxygen, fits in with an oxidation-reduction mechanism. The sulfur-oxygen radical species, which appear when oxygen is admitted to sulfur radicals, are assigned to sulfur chains containing one or two oxygen atoms at the end of the chain. It is very likely that these sulfur-oxygen radicals are intermediates in the proposed mechanism. The formation of the byproduct SO2 from SxO2 · − at temperatures above 175 °C is also visible in the ESR spectrum. On the basis of the experiments it is concluded that in the mechanism of H2S oxidation on active carbons, carbon radicals do not play an important role.

AB - ESR experiments on the oxidation of hydrogen sulfide were performed in the temperature range 20–150 °C. Alumina, active carbon and molecular sieve zeolite 13X were investigated as catalysts. For zeolite 13X it was demonstrated that the reaction is autocatalytic and that sulfur radicals are the active sites for oxygen chemisorption. The intensity of the sulfur radical ESR signal, which is related to the degree of conversion of these radicals, by oxygen, fits in with an oxidation-reduction mechanism. The sulfur-oxygen radical species, which appear when oxygen is admitted to sulfur radicals, are assigned to sulfur chains containing one or two oxygen atoms at the end of the chain. It is very likely that these sulfur-oxygen radicals are intermediates in the proposed mechanism. The formation of the byproduct SO2 from SxO2 · − at temperatures above 175 °C is also visible in the ESR spectrum. On the basis of the experiments it is concluded that in the mechanism of H2S oxidation on active carbons, carbon radicals do not play an important role.

KW - IR-68342

U2 - 10.1016/0021-9517(76)90095-6

DO - 10.1016/0021-9517(76)90095-6

M3 - Article

VL - 42

SP - 96

EP - 106

JO - Journal of catalysis

JF - Journal of catalysis

SN - 0021-9517

IS - 1

ER -