Impact of support oxide acidity in Pt-catalyzed HMF hydrogenation in alcoholic medium

Nhu Ly, Katharina Al-Shamery, Carine E. Chan-Thaw, Laura Prati, Paolo Carniti, Antonella Gervasini*

*Kontaktforfatter for dette arbejde

Publikation: Bidrag til tidsskriftTidsskriftartikelForskningpeer review

Resumé

Abstract: Silica and three mixed silica oxides (silica–alumina, silica–niobia, and silica–zirconia) with nominally 5 wt% of the added element (Al, Nb and Zr) were prepared and used as supports for dispersing monometallic Pt-nanoparticles. The presence of the second oxide component on the silica surface influenced some properties of the final samples, like surface area and acidity. The samples acidity was measured in a recirculation adsorption line with 2-phenylethylamine probe, by performing the titrations both in cyclohexane and in methanol to gather the intrinsic and effective acidity, respectively. The acid site density of silica–alumina was the highest compared with the other oxides; in general, an important decrease of acid sites density was determined in methanol. The order of the effective acidity in methanol was different from that determined in cyclohexane only for silica–zirconia and silica–niobia, confirming the peculiar acidity of Nb-oxide compounds in polar liquids: Colloidal spherical platinum nanoparticles were synthesized and then deposited (1 wt%) on the oxide supports. The obtained metallic nanophases were studied in the reduction of 5-hydroxymethylfurfural (HMF) to valuable chemicals such as dimethylfuran, dimethyltetrahydro-furan, 2-hexanol. In particular, this study focused on the impact of the acidity of the oxide supports on reaction selectivity when 2-butanol is used as solvent. When Pt is not present, Nb-doped silica is the most effective catalyst to di-hydroxymethyl furan diether (DHMFDE) derived from Meerwein–Ponndorf–Verley reaction, maintaining its Lewis character also in protic medium. In the presence of Pt, Nb-doped silica, however, presents the higher selectivity to hydrogenolysis products, 5-methyl furan (5-MF). Graphical Abstract: [Figure not available: see fulltext.]

OriginalsprogEngelsk
TidsskriftCatalysis Letters
Vol/bind147
Udgave nummer2
Sider (fra-til)345-359
ISSN1011-372X
DOI
StatusUdgivet - 2017
Udgivet eksterntJa

Fingeraftryk

Acidity
Oxides
Hydrogenation
Silicon Dioxide
Silica
Methanol
Cyclohexane
Nanoparticles
Hydrogenolysis
Acids
Platinum
Butenes
Titration
5-hydroxymethylfurfural
Adsorption
Catalysts
Liquids
furan

Citer dette

Ly, Nhu ; Al-Shamery, Katharina ; Chan-Thaw, Carine E. ; Prati, Laura ; Carniti, Paolo ; Gervasini, Antonella. / Impact of support oxide acidity in Pt-catalyzed HMF hydrogenation in alcoholic medium. I: Catalysis Letters. 2017 ; Bind 147, Nr. 2. s. 345-359.
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title = "Impact of support oxide acidity in Pt-catalyzed HMF hydrogenation in alcoholic medium",
abstract = "Abstract: Silica and three mixed silica oxides (silica–alumina, silica–niobia, and silica–zirconia) with nominally 5 wt{\%} of the added element (Al, Nb and Zr) were prepared and used as supports for dispersing monometallic Pt-nanoparticles. The presence of the second oxide component on the silica surface influenced some properties of the final samples, like surface area and acidity. The samples acidity was measured in a recirculation adsorption line with 2-phenylethylamine probe, by performing the titrations both in cyclohexane and in methanol to gather the intrinsic and effective acidity, respectively. The acid site density of silica–alumina was the highest compared with the other oxides; in general, an important decrease of acid sites density was determined in methanol. The order of the effective acidity in methanol was different from that determined in cyclohexane only for silica–zirconia and silica–niobia, confirming the peculiar acidity of Nb-oxide compounds in polar liquids: Colloidal spherical platinum nanoparticles were synthesized and then deposited (1 wt{\%}) on the oxide supports. The obtained metallic nanophases were studied in the reduction of 5-hydroxymethylfurfural (HMF) to valuable chemicals such as dimethylfuran, dimethyltetrahydro-furan, 2-hexanol. In particular, this study focused on the impact of the acidity of the oxide supports on reaction selectivity when 2-butanol is used as solvent. When Pt is not present, Nb-doped silica is the most effective catalyst to di-hydroxymethyl furan diether (DHMFDE) derived from Meerwein–Ponndorf–Verley reaction, maintaining its Lewis character also in protic medium. In the presence of Pt, Nb-doped silica, however, presents the higher selectivity to hydrogenolysis products, 5-methyl furan (5-MF). Graphical Abstract: [Figure not available: see fulltext.]",
keywords = "HMF hydrogenation, Intrinsic and Effective acidity, Modified silica oxides, Pt nanoparticles",
author = "Nhu Ly and Katharina Al-Shamery and Chan-Thaw, {Carine E.} and Laura Prati and Paolo Carniti and Antonella Gervasini",
year = "2017",
doi = "10.1007/s10562-016-1945-9",
language = "English",
volume = "147",
pages = "345--359",
journal = "Catalysis Letters",
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Impact of support oxide acidity in Pt-catalyzed HMF hydrogenation in alcoholic medium. / Ly, Nhu; Al-Shamery, Katharina; Chan-Thaw, Carine E.; Prati, Laura; Carniti, Paolo; Gervasini, Antonella.

I: Catalysis Letters, Bind 147, Nr. 2, 2017, s. 345-359.

Publikation: Bidrag til tidsskriftTidsskriftartikelForskningpeer review

TY - JOUR

T1 - Impact of support oxide acidity in Pt-catalyzed HMF hydrogenation in alcoholic medium

AU - Ly, Nhu

AU - Al-Shamery, Katharina

AU - Chan-Thaw, Carine E.

AU - Prati, Laura

AU - Carniti, Paolo

AU - Gervasini, Antonella

PY - 2017

Y1 - 2017

N2 - Abstract: Silica and three mixed silica oxides (silica–alumina, silica–niobia, and silica–zirconia) with nominally 5 wt% of the added element (Al, Nb and Zr) were prepared and used as supports for dispersing monometallic Pt-nanoparticles. The presence of the second oxide component on the silica surface influenced some properties of the final samples, like surface area and acidity. The samples acidity was measured in a recirculation adsorption line with 2-phenylethylamine probe, by performing the titrations both in cyclohexane and in methanol to gather the intrinsic and effective acidity, respectively. The acid site density of silica–alumina was the highest compared with the other oxides; in general, an important decrease of acid sites density was determined in methanol. The order of the effective acidity in methanol was different from that determined in cyclohexane only for silica–zirconia and silica–niobia, confirming the peculiar acidity of Nb-oxide compounds in polar liquids: Colloidal spherical platinum nanoparticles were synthesized and then deposited (1 wt%) on the oxide supports. The obtained metallic nanophases were studied in the reduction of 5-hydroxymethylfurfural (HMF) to valuable chemicals such as dimethylfuran, dimethyltetrahydro-furan, 2-hexanol. In particular, this study focused on the impact of the acidity of the oxide supports on reaction selectivity when 2-butanol is used as solvent. When Pt is not present, Nb-doped silica is the most effective catalyst to di-hydroxymethyl furan diether (DHMFDE) derived from Meerwein–Ponndorf–Verley reaction, maintaining its Lewis character also in protic medium. In the presence of Pt, Nb-doped silica, however, presents the higher selectivity to hydrogenolysis products, 5-methyl furan (5-MF). Graphical Abstract: [Figure not available: see fulltext.]

AB - Abstract: Silica and three mixed silica oxides (silica–alumina, silica–niobia, and silica–zirconia) with nominally 5 wt% of the added element (Al, Nb and Zr) were prepared and used as supports for dispersing monometallic Pt-nanoparticles. The presence of the second oxide component on the silica surface influenced some properties of the final samples, like surface area and acidity. The samples acidity was measured in a recirculation adsorption line with 2-phenylethylamine probe, by performing the titrations both in cyclohexane and in methanol to gather the intrinsic and effective acidity, respectively. The acid site density of silica–alumina was the highest compared with the other oxides; in general, an important decrease of acid sites density was determined in methanol. The order of the effective acidity in methanol was different from that determined in cyclohexane only for silica–zirconia and silica–niobia, confirming the peculiar acidity of Nb-oxide compounds in polar liquids: Colloidal spherical platinum nanoparticles were synthesized and then deposited (1 wt%) on the oxide supports. The obtained metallic nanophases were studied in the reduction of 5-hydroxymethylfurfural (HMF) to valuable chemicals such as dimethylfuran, dimethyltetrahydro-furan, 2-hexanol. In particular, this study focused on the impact of the acidity of the oxide supports on reaction selectivity when 2-butanol is used as solvent. When Pt is not present, Nb-doped silica is the most effective catalyst to di-hydroxymethyl furan diether (DHMFDE) derived from Meerwein–Ponndorf–Verley reaction, maintaining its Lewis character also in protic medium. In the presence of Pt, Nb-doped silica, however, presents the higher selectivity to hydrogenolysis products, 5-methyl furan (5-MF). Graphical Abstract: [Figure not available: see fulltext.]

KW - HMF hydrogenation

KW - Intrinsic and Effective acidity

KW - Modified silica oxides

KW - Pt nanoparticles

U2 - 10.1007/s10562-016-1945-9

DO - 10.1007/s10562-016-1945-9

M3 - Journal article

AN - SCOPUS:85007478259

VL - 147

SP - 345

EP - 359

JO - Catalysis Letters

JF - Catalysis Letters

SN - 1011-372X

IS - 2

ER -