Adsorption of H2S on alumina at low coverages

deRosset, A.J.; Finstrom, C.G.; Adams, Chris J.

doi:10.1016/0021-9517(62)90052-0

Cited by 22 publications

(3 citation statements)

References 8 publications

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“…The surfaces of the particles are typically inhomogeneous, owing to the presence of surface defects, multiple hydroxyl groups, and different crystalline faces that terminate the surface. Transmission infrared spectroscopy can be applied to help characterize these surfaces by resolving different hydroxyl group stretching modes − and adsorbate vibrations on different adsorption sites. − For example, by employing CO as an adsorbate on the Al 2 O 3 surface, Zaki and Knözinger were able to distinguish acidic and basic OH groups 9 and octahedrally and tetrahedrally bound Al 3+ sites . Using CO as a probe molecule, Ballinger and Yates were able to correlate the formation of two different types of Al 3+ sites with the thermal removal of the hydroxyl groups …”

Section: Introductionmentioning

confidence: 99%

Infrared Spectroscopic Study of Surface Diffusion to Surface Hydroxyl Groups on Al₂O₃: 2-Chloroethylethyl Sulfide Adsorption Site Selection

et al. 2000

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The interaction of the various hydroxyl groups on the Al2O3 surface with a bifunctional adsorbate, 2-chloroethylethyl sulfide, was studied by transmission infrared spectroscopy. Al2O3 has five unique Al-OH groups, differentiated by their coordination to the surface, which give independent AlO-H stretching modes. Monitoring intensity changes in these modes as 2-chloroethylethyl sulfide (CEES) molecules diffuse into the porous structure of alumina shows distinctly different stages of surface diffusion and reaction at the Al-OH groups. Three sequential steps have been separated by studies at low temperature, where the rate of the processes was kinetically retarded to allow observation. The final stage of the CEES interaction with the surface occur when the CEES molecules adsorbed on the surface via the sulfide moiety at Al 3+ Lewis acid sites undergo a hydrolysis reaction with the neighboring basic Al-OH groups.

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Section: Introductionmentioning

confidence: 99%

Infrared Spectroscopic Study of Surface Diffusion to Surface Hydroxyl Groups on Al₂O₃: 2-Chloroethylethyl Sulfide Adsorption Site Selection

et al. 2000

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“…18,19 It would be advantageous to understand the detailed reaction process between g-Al 2 O 3 surface and H 2 S. Research on this surface reaction may be helpful to improve performance of desulfurizers. DeRosset et al 26 estimated that isosteric heats of adsorption of H 2 S ranged from À104.6 to À159.0 kJ mol À1 , depending on the degree of dehydration of the g-Al 2 O 3 . 15,[20][21][22][23][24] For example, Travert et al studied interaction of H 2 S on g-Al 2 O 3 surface using infrared (IR) spectroscopy, 25 and showed that the adsorption of H 2 S irreversibly perturbs the high-frequency region of the IR spectroscopy and results in changes to surface acidity.…”

Section: Introductionmentioning

confidence: 99%

“…15,[20][21][22][23][24] For example, Travert et al studied interaction of H 2 S on g-Al 2 O 3 surface using infrared (IR) spectroscopy, 25 and showed that the adsorption of H 2 S irreversibly perturbs the high-frequency region of the IR spectroscopy and results in changes to surface acidity. DeRosset et al 26 estimated that isosteric heats of adsorption of H 2 S ranged from À104.6 to À159.0 kJ mol À1 , depending on the degree of dehydration of the g-Al 2 O 3 . And entropy calculations indicate that mobility of the adsorbed H 2 S is highly restricted.…”

Section: Introductionmentioning

confidence: 99%

Theoretical investigation of H₂S removal on γ-Al₂O₃ surfaces of different hydroxyl coverage

et al. 2015

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The sulfurized processes of H 2 S on dehydrated (100) and (110) as well as partially hydrated (110) surfaces of g-Al 2 O 3 were investigated using a periodic density functional theory method. The adsorption configurations of possible intermediates and the potential energy profiles of reaction are depicted. Our results show that H 2 S adsorbs preferentially on the Al site along with the S bond, and the adsorption energies are À32.52 and À114.38 kJ mol À1 on the dehydrated (100) and (110) surfaces, respectively. As the reaction temperature of the desulfurization changes, the (110) surface presents different levels of hydroxyl coverage, which affects the adsorption structures of species and reaction energies of dissociation processes. The bonding strengths of H 2 S on the partially hydrated (110) surfaces are weaker than on the dehydrated (110) surface. Compared with the 3.0 and 8.9 OH per nm 2 surfaces, the H 2 S has the weakest adsorption energy (À39.85 kJ mol À1 ) and the highest activation energy (92.06 kJ mol À1 ) on the 5.9 OH per nm 2 surface. On the 8.9 OH per nm 2 surface, the activation energy of the second dissociation step (rate-determining step) for H 2 S dissociation is merely 38.32 kJ mol À1 . On these involved surfaces, cleavage processes of the two H-S bonds present facile activation energies, which are facilitative to desulfurization. View Article Onlinea Param: parameters. b D100, the dehydrated g-Al 2 O 3 (100) surface. c D110, the dehydrated g-Al 2 O 3 (110) surface. d FS denotes the nal state. e 3.0 OH per nm 2 , 5.9 OH per nm 2 and 8.9 OH per nm 2 represent the different levels of hydroxyl coverage for g-Al 2 O 3 (110) surface. This journal isFig. 6 Calculated probable potential energy profiles for dissociation of H 2 S (a) and HS (b) on dehydrated and partially hydrated g-Al 2 O 3 surfaces. (D100 surface, the dehydrated g-Al 2 O 3 (100) surface; D110 surface, the dehydrated g-Al 2 O 3 (110) surface).This journal is

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Adsorption of H2S on alumina at low coverages

Cited by 22 publications

References 8 publications

Infrared Spectroscopic Study of Surface Diffusion to Surface Hydroxyl Groups on Al₂O₃: 2-Chloroethylethyl Sulfide Adsorption Site Selection

Infrared Spectroscopic Study of Surface Diffusion to Surface Hydroxyl Groups on Al₂O₃: 2-Chloroethylethyl Sulfide Adsorption Site Selection

Theoretical investigation of H₂S removal on γ-Al₂O₃ surfaces of different hydroxyl coverage

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Adsorption of H2S on alumina at low coverages

Cited by 22 publications

References 8 publications

Infrared Spectroscopic Study of Surface Diffusion to Surface Hydroxyl Groups on Al2O3: 2-Chloroethylethyl Sulfide Adsorption Site Selection

Infrared Spectroscopic Study of Surface Diffusion to Surface Hydroxyl Groups on Al2O3: 2-Chloroethylethyl Sulfide Adsorption Site Selection

Theoretical investigation of H2S removal on γ-Al2O3 surfaces of different hydroxyl coverage

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Infrared Spectroscopic Study of Surface Diffusion to Surface Hydroxyl Groups on Al₂O₃: 2-Chloroethylethyl Sulfide Adsorption Site Selection

Infrared Spectroscopic Study of Surface Diffusion to Surface Hydroxyl Groups on Al₂O₃: 2-Chloroethylethyl Sulfide Adsorption Site Selection

Theoretical investigation of H₂S removal on γ-Al₂O₃ surfaces of different hydroxyl coverage