Reduction of SO2 on different carbons

Humeres, Eduardo; Moreira, Regina de Fátima Peralta Muniz; Peruch, Maria da Gloria B.

doi:10.1016/s0008-6223(01)00193-2

Cited by 55 publications

(79 citation statements)

References 15 publications

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“…There were no complaints about CS 2 odor at ground level near the plant during our measurements. (2) Carbon disulfide might be formed in the late state of the combustion of sulfur containing fuels by the following overall sequence of reactions [ Bejarano et al , 2001; Clark et al , 2001; Humeres et al , 2002]:

…”

Section: Resultsmentioning

confidence: 99%

“…The reactions would be heterogeneous between gaseous and solid components. The above sequence of reactions and has been suggested and investigated for flue gas desulfurization [see Bejarano et al , 2001; Clark et al , 2001; Humeres et al , 2002 and references therein]. Both authors find formation of CS 2 and COS at elevated temperatures (above about 700°C), and at even higher temperatures (>800°C) CS 2 would be the major product [ Bejarano et al , 2001].…”

Section: Resultsmentioning

confidence: 99%

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Observations of carbon disulfide by differential optical absorption spectroscopy in Shanghai

Geyer

Xie

et al. 2004

Geophysical Research Letters

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Carbon disulfide, CS2, is an important sulfur‐containing species in the global environment. Its oxidation to SO2 and COS are basic atmospheric chemical processes in the sulfur cycle. The typical measurement methods for CS2 are gas chromatography with flame photometric detection (GC‐FPD) and gas chromatography ‐ mass spectrometry (GC‐MS). This paper presents CS2 and SO2 long‐term measurements made by the long path Differential Optical Absorption Spectroscopy (DOAS) technique in the winter of 2001 to 2002 in the urban area of Shanghai, China. We found a good correlation between SO2 and CS2 with average [SO2]/[CS2] ≈ 2.1. Combined with an analysis of pollution sources near the measurement site, our measurements indicate that CS2 came mainly from a coal burning furnace close to the measurement site.

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…”

Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

Observations of carbon disulfide by differential optical absorption spectroscopy in Shanghai

Geyer

Xie

et al. 2004

Geophysical Research Letters

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“…The study of (C + SO 2 ) reaction on different carbons (graphite, charcoal, activated carbon, cokes, and graphene oxide (MPGO)) showed that the reaction proceeds through the same stoichiometry for all carbons (Eqn 1), while the reactivity increases with decreasing crystallinity and increasing oxygen content. [1][2][3][4] SO 2 þ C→ CO 2 þ 1 = 2 S 2 (1) Experimental data obtained from SO 2 reduction on carbons along with theoretical calculations [5] allowed a detailed description of the primary reaction ( Fig. 1), where the diradical zigzag fragment represents the site of insertion of SO 2 in the carbon matrix.…”

Section: Introductionmentioning

confidence: 99%

Interconversion and selective reactivity of sulfur dioxide reduction intermediates inserted on graphene oxide

Smaniotto

Humeres

Debacher

et al. 2016

J of Physical Organic Chem

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Graphene oxide, MPGO, was obtained by oxidation of graphite microparticles by a H 2 SO 4 /KMnO 4 /H 2 O 2 mixture followed by thermal exfoliation. Non-thermal plasma treatment of MPGO under SO 2 atmosphere resulted in the insertion of the oxidized intermediates only. Refluxing this material in CS 2 (46°C) showed sulfur elimination and interconversion of the oxidized into non-oxidized intermediates with an energetic barrier of ΔG ‡ = 25.81 kcal mol À1 without decarboxylation. The episulfide content in modified MPGO increases with respect to the oxidized intermediates when increasing temperature. Modification of MPGO with SO 2 at 630°C presented exclusively the non-oxidized intermediate. These results support the hypothesis that there are two major reactions with different energetic demand in the SO 2 reduction on carbons: desulfurization and decarboxylation. The selectivity of thiolysis and aminolysis towards the intermediates inserted in the MPGO matrix allowed the aminothiolysis of a sample containing both intermediates with the insertion of the amino group on the episulfide site followed by an intramolecular thiolysis with double functionalization of the matrix.

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“…In this review we describe the methodology used to study the mechanism of a solid–gas reaction in a flow reactor and the necessary conditions that allowed to measure the conversion of the solid and the product distribution when the kinetics was chemically controlled …”

Section: Introductionmentioning

confidence: 99%

Kinetics and mechanisms in flow systems: reduction of SO₂ on carbons

Humeres

Moreira

2012

J of Physical Organic Chem

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Surface‐science studies of some reactions have allowed postulating the mechanisms using a variety of techniques. The surface chemistry of Group IV elements has been particularly studied recently because Si, Ge, and C are semiconductors, and the surface organic chemistry to functionalize these elements has seen immense progress in recent years. In this review article we describe the methodology used to study the mechanism of a solid–gas reaction, the reduction of SO2 on carbons, and the necessary conditions that allowed the measurement of the solid conversion and product distribution when the kinetics was chemically controlled and the reaction had reached the steady state. The reaction was first‐order with respect to SO2 and with respect to carbon and the stoichiometry was determined from the product distribution. The reaction proceeds through two thermally stable reaction intermediates bound to the surface, a six‐membered ring 1,3,2‐dioxathiolane and a five‐membered ring 1,2‐oxathietene 2‐oxide or γ‐sultine, both species being in equilibrium. The reaction was shown to be reversible. The primary product is an episulfide that, after a series of consecutive reactions of atomic sulfur, is able to free sulfur. The reactivity of the intermediates and the episulfide was studied for several reactions and consistent mechanisms were postulated from the X‐ray photoelectron spectroscopy and solid state nuclear magnetic resonance spectra. Aminolysis and the reaction with alkyl halides resulted on the insertion of the alkyl moiety in the episulfide primary product, while the thiolysis and photolytic alcoholysis resulted in the insertion of the alkyl moiety in the oxidized intermediates. Copyright © 2012 John Wiley & Sons, Ltd.

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Reduction of SO2 on different carbons

Cited by 55 publications

References 15 publications

Observations of carbon disulfide by differential optical absorption spectroscopy in Shanghai

Observations of carbon disulfide by differential optical absorption spectroscopy in Shanghai

Interconversion and selective reactivity of sulfur dioxide reduction intermediates inserted on graphene oxide

Kinetics and mechanisms in flow systems: reduction of SO₂ on carbons

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Reduction of SO2 on different carbons

Cited by 55 publications

References 15 publications

Observations of carbon disulfide by differential optical absorption spectroscopy in Shanghai

Observations of carbon disulfide by differential optical absorption spectroscopy in Shanghai

Interconversion and selective reactivity of sulfur dioxide reduction intermediates inserted on graphene oxide

Kinetics and mechanisms in flow systems: reduction of SO2 on carbons

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Product

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Kinetics and mechanisms in flow systems: reduction of SO₂ on carbons