The nature of the sulfur tolerance of amorphous silica-alumina supported NiMo(W) sulfide and Pt hydrogenation catalysts

A.E. Coumans, D.G. Poduval, J.A.R. Veen, van, E.J.M. Hensen

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Abstract

Amorphous silica-alumina (ASA) based NiMo and NiW sulfide and Pt hydrogenation catalysts were prepared and compared in toluene hydrogenation in the presence of H2S to alumina- and silica-supported reference catalysts with the aim to elucidate the influence of (strong) Brønsted acidity of the support on the sulfur tolerance. Despite precautions to prepare NiMo sulfide catalysts with equal morphology, the stacking degree of the MoS2 phase was found to decrease with alumina content of the ASA. Similar but more pronounced differences of the stacking degree were observed among the NiW sulfide catalysts. This variation in the stacking degree had a substantial effect on the catalytic activity of dibenzothiophene hydrodesulfurization. ASA-based catalysts show higher activity and improved sulfur tolerance in toluene hydrogenation compared to their alumina- and silica based counterparts. However, the sulfur tolerance does not correlate with the number of strong Brønsted acid sites, nor, indeed, with total Brønsted acidity. Instead, it decreases with increasing Al content of the ASA support. The sulfur tolerance of the active metal sulfide phase is related to the electronegativity of the support. That silica itself does not follow this trend is surmised to be due to its lack of Lewis acid sites, necessary for introducing the active phase-support effect.
Original languageEnglish
Pages (from-to)51-59
Number of pages9
JournalApplied Catalysis. A, General
Volume411-412
DOIs
Publication statusPublished - 2012

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Aluminum Oxide
Sulfides
Sulfur
Silicon Dioxide
Hydrogenation
Alumina
Silica
Catalysts
Toluene
Acidity
Lewis Acids
Electronegativity
Hydrodesulfurization
Acids
Catalyst activity
Metals

Cite this

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title = "The nature of the sulfur tolerance of amorphous silica-alumina supported NiMo(W) sulfide and Pt hydrogenation catalysts",
abstract = "Amorphous silica-alumina (ASA) based NiMo and NiW sulfide and Pt hydrogenation catalysts were prepared and compared in toluene hydrogenation in the presence of H2S to alumina- and silica-supported reference catalysts with the aim to elucidate the influence of (strong) Br{\o}nsted acidity of the support on the sulfur tolerance. Despite precautions to prepare NiMo sulfide catalysts with equal morphology, the stacking degree of the MoS2 phase was found to decrease with alumina content of the ASA. Similar but more pronounced differences of the stacking degree were observed among the NiW sulfide catalysts. This variation in the stacking degree had a substantial effect on the catalytic activity of dibenzothiophene hydrodesulfurization. ASA-based catalysts show higher activity and improved sulfur tolerance in toluene hydrogenation compared to their alumina- and silica based counterparts. However, the sulfur tolerance does not correlate with the number of strong Br{\o}nsted acid sites, nor, indeed, with total Br{\o}nsted acidity. Instead, it decreases with increasing Al content of the ASA support. The sulfur tolerance of the active metal sulfide phase is related to the electronegativity of the support. That silica itself does not follow this trend is surmised to be due to its lack of Lewis acid sites, necessary for introducing the active phase-support effect.",
author = "A.E. Coumans and D.G. Poduval and {Veen, van}, J.A.R. and E.J.M. Hensen",
year = "2012",
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language = "English",
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The nature of the sulfur tolerance of amorphous silica-alumina supported NiMo(W) sulfide and Pt hydrogenation catalysts. / Coumans, A.E.; Poduval, D.G.; Veen, van, J.A.R.; Hensen, E.J.M.

In: Applied Catalysis. A, General, Vol. 411-412, 2012, p. 51-59.

Research output: Contribution to journalArticleAcademicpeer-review

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T1 - The nature of the sulfur tolerance of amorphous silica-alumina supported NiMo(W) sulfide and Pt hydrogenation catalysts

AU - Coumans, A.E.

AU - Poduval, D.G.

AU - Veen, van, J.A.R.

AU - Hensen, E.J.M.

PY - 2012

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N2 - Amorphous silica-alumina (ASA) based NiMo and NiW sulfide and Pt hydrogenation catalysts were prepared and compared in toluene hydrogenation in the presence of H2S to alumina- and silica-supported reference catalysts with the aim to elucidate the influence of (strong) Brønsted acidity of the support on the sulfur tolerance. Despite precautions to prepare NiMo sulfide catalysts with equal morphology, the stacking degree of the MoS2 phase was found to decrease with alumina content of the ASA. Similar but more pronounced differences of the stacking degree were observed among the NiW sulfide catalysts. This variation in the stacking degree had a substantial effect on the catalytic activity of dibenzothiophene hydrodesulfurization. ASA-based catalysts show higher activity and improved sulfur tolerance in toluene hydrogenation compared to their alumina- and silica based counterparts. However, the sulfur tolerance does not correlate with the number of strong Brønsted acid sites, nor, indeed, with total Brønsted acidity. Instead, it decreases with increasing Al content of the ASA support. The sulfur tolerance of the active metal sulfide phase is related to the electronegativity of the support. That silica itself does not follow this trend is surmised to be due to its lack of Lewis acid sites, necessary for introducing the active phase-support effect.

AB - Amorphous silica-alumina (ASA) based NiMo and NiW sulfide and Pt hydrogenation catalysts were prepared and compared in toluene hydrogenation in the presence of H2S to alumina- and silica-supported reference catalysts with the aim to elucidate the influence of (strong) Brønsted acidity of the support on the sulfur tolerance. Despite precautions to prepare NiMo sulfide catalysts with equal morphology, the stacking degree of the MoS2 phase was found to decrease with alumina content of the ASA. Similar but more pronounced differences of the stacking degree were observed among the NiW sulfide catalysts. This variation in the stacking degree had a substantial effect on the catalytic activity of dibenzothiophene hydrodesulfurization. ASA-based catalysts show higher activity and improved sulfur tolerance in toluene hydrogenation compared to their alumina- and silica based counterparts. However, the sulfur tolerance does not correlate with the number of strong Brønsted acid sites, nor, indeed, with total Brønsted acidity. Instead, it decreases with increasing Al content of the ASA support. The sulfur tolerance of the active metal sulfide phase is related to the electronegativity of the support. That silica itself does not follow this trend is surmised to be due to its lack of Lewis acid sites, necessary for introducing the active phase-support effect.

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