New sulfur adsorbents derived from layered double hydroxides. II. DRIFTS study of COS and H2S adsorption

Todd J. Toops; Mark Crocker

doi:10.1016/j.apcatb.2008.01.013

New sulfur adsorbents derived from layered double hydroxides. II. DRIFTS study of COS and H₂S adsorption

Todd J. Toops, Mark Crocker

Chemistry

Research output: Contribution to journal › Article › peer-review

59 Scopus citations

Abstract

H₂S and COS adsorption were studied on two calcined layered double hydroxides (LDHs), Mg_0.75Al_0.25(OH)₂(CO₃)_0.125 and Mg_0.65Al_0.35(OH)₂(CO₃)_0.175, using diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and a chemisorption apparatus. Both demonstrated the ability to irreversibly adsorb H₂S, corresponding to uptakes of 1.54 and 1.76 μmol/m², respectively, but Mg_0.75Al_0.25 had a significantly larger capacity for COS, 1.62 μmol/m² compared to 0.80 μmol/m² for Mg_0.65Al_0.35. Analysis of the DRIFT spectra suggests the adsorption of H₂S proceeds via the substitution of lattice oxygen with sulfur, resulting in the formation of H₂O on the surface. COS adsorption is more complicated, although it appears that a similar substitution of lattice oxygen with sulfur occurs. This results in the formation of CO₂ and subsequently bicarbonates and carbonates. The formation of hydrogen thiocarbonate is also involved, although this form is generally only observed in the later stages of adsorption and appears to form at the expense of bicarbonate. The Mg_0.75Al_0.25 LDH retained its ability to adsorb COS in the presence of propene.

Original language	English
Pages (from-to)	199-207
Number of pages	9
Journal	Applied Catalysis B: Environmental
Volume	82
Issue number	3-4
DOIs	https://doi.org/10.1016/j.apcatb.2008.01.013
State	Published - Aug 8 2008

Keywords

Adsorption
Carbonyl sulfide
DRIFTS
Hydrotalcite
Layered double hydroxide

ASJC Scopus subject areas

Catalysis
General Environmental Science
Process Chemistry and Technology

Access to Document

10.1016/j.apcatb.2008.01.013

Cite this

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title = "New sulfur adsorbents derived from layered double hydroxides. II. DRIFTS study of COS and H2S adsorption",

abstract = "H2S and COS adsorption were studied on two calcined layered double hydroxides (LDHs), Mg0.75Al0.25(OH)2(CO3)0.125 and Mg0.65Al0.35(OH)2(CO3)0.175, using diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and a chemisorption apparatus. Both demonstrated the ability to irreversibly adsorb H2S, corresponding to uptakes of 1.54 and 1.76 μmol/m2, respectively, but Mg0.75Al0.25 had a significantly larger capacity for COS, 1.62 μmol/m2 compared to 0.80 μmol/m2 for Mg0.65Al0.35. Analysis of the DRIFT spectra suggests the adsorption of H2S proceeds via the substitution of lattice oxygen with sulfur, resulting in the formation of H2O on the surface. COS adsorption is more complicated, although it appears that a similar substitution of lattice oxygen with sulfur occurs. This results in the formation of CO2 and subsequently bicarbonates and carbonates. The formation of hydrogen thiocarbonate is also involved, although this form is generally only observed in the later stages of adsorption and appears to form at the expense of bicarbonate. The Mg0.75Al0.25 LDH retained its ability to adsorb COS in the presence of propene.",

keywords = "Adsorption, Carbonyl sulfide, DRIFTS, Hydrotalcite, Layered double hydroxide",

author = "Toops, {Todd J.} and Mark Crocker",

year = "2008",

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doi = "10.1016/j.apcatb.2008.01.013",

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T1 - New sulfur adsorbents derived from layered double hydroxides. II. DRIFTS study of COS and H2S adsorption

AU - Toops, Todd J.

AU - Crocker, Mark

PY - 2008/8/8

Y1 - 2008/8/8

N2 - H2S and COS adsorption were studied on two calcined layered double hydroxides (LDHs), Mg0.75Al0.25(OH)2(CO3)0.125 and Mg0.65Al0.35(OH)2(CO3)0.175, using diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and a chemisorption apparatus. Both demonstrated the ability to irreversibly adsorb H2S, corresponding to uptakes of 1.54 and 1.76 μmol/m2, respectively, but Mg0.75Al0.25 had a significantly larger capacity for COS, 1.62 μmol/m2 compared to 0.80 μmol/m2 for Mg0.65Al0.35. Analysis of the DRIFT spectra suggests the adsorption of H2S proceeds via the substitution of lattice oxygen with sulfur, resulting in the formation of H2O on the surface. COS adsorption is more complicated, although it appears that a similar substitution of lattice oxygen with sulfur occurs. This results in the formation of CO2 and subsequently bicarbonates and carbonates. The formation of hydrogen thiocarbonate is also involved, although this form is generally only observed in the later stages of adsorption and appears to form at the expense of bicarbonate. The Mg0.75Al0.25 LDH retained its ability to adsorb COS in the presence of propene.

AB - H2S and COS adsorption were studied on two calcined layered double hydroxides (LDHs), Mg0.75Al0.25(OH)2(CO3)0.125 and Mg0.65Al0.35(OH)2(CO3)0.175, using diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and a chemisorption apparatus. Both demonstrated the ability to irreversibly adsorb H2S, corresponding to uptakes of 1.54 and 1.76 μmol/m2, respectively, but Mg0.75Al0.25 had a significantly larger capacity for COS, 1.62 μmol/m2 compared to 0.80 μmol/m2 for Mg0.65Al0.35. Analysis of the DRIFT spectra suggests the adsorption of H2S proceeds via the substitution of lattice oxygen with sulfur, resulting in the formation of H2O on the surface. COS adsorption is more complicated, although it appears that a similar substitution of lattice oxygen with sulfur occurs. This results in the formation of CO2 and subsequently bicarbonates and carbonates. The formation of hydrogen thiocarbonate is also involved, although this form is generally only observed in the later stages of adsorption and appears to form at the expense of bicarbonate. The Mg0.75Al0.25 LDH retained its ability to adsorb COS in the presence of propene.

KW - Adsorption

KW - Carbonyl sulfide

KW - DRIFTS

KW - Hydrotalcite

KW - Layered double hydroxide

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