Factors influencing the catalytic oxidation of benzyl alcohol using supported phosphine-capped gold nanoparticles

Rohul Adnan; Gunther Andersson; Matthew Polson; Gregory Metha; Vladimir Golovko

doi:10.1039/c4cy01168f

Factors influencing the catalytic oxidation of benzyl alcohol using supported phosphine-capped gold nanoparticles

Rohul Adnan, Gunther Andersson, Matthew Polson, Gregory Metha, Vladimir Golovko

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

67 Citations (Scopus)

Abstract

Two phosphine-stabilised gold clusters, Au₁₀₁(PPh₃)₂₁Cl₅ and Au₉(PPh₃)₈(NO₃)₃, were deposited and activated on anatase TiO₂ and fumed SiO₂. These catalysts showed an almost complete oxidation of benzyl alcohol (>90%) within 3 hours at 80 °C and 3 bar O₂ in methanol with a high substrate-to-metal molar ratio of 5800 and turn-over frequency of 0.65 s^-1. Factors influencing catalytic activity were investigated, including metal-support interaction, effects of heat treatments, chemical composition of gold clusters, the size of gold nanoparticles and catalytic conditions. It was found that the anions present in gold clusters play a role in determining the catalytic activity in this reaction, with NO₃^- diminishing the catalytic activity. High catalytic activity was attributed to the formation of large gold nanoparticles (>2 nm) that coincides with partial removal of ligands which occurs during heat treatment and catalysis. Selectivity towards the formation of methyl benzoate can be tuned by selection of the reaction temperature. The catalysts were characterised using transmission electron microscopy, UV-vis diffuse reflectance spectroscopy and X-ray photoelectron spectroscopy.

Original language	English
Pages (from-to)	1323-1333
Number of pages	11
Journal	Catalysis Science and Technology
Volume	5
Issue number	2
DOIs	https://doi.org/10.1039/c4cy01168f
Publication status	Published - 1 Feb 2015

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title = "Factors influencing the catalytic oxidation of benzyl alcohol using supported phosphine-capped gold nanoparticles",

abstract = "Two phosphine-stabilised gold clusters, Au101(PPh3)21Cl5 and Au9(PPh3)8(NO3)3, were deposited and activated on anatase TiO2 and fumed SiO2. These catalysts showed an almost complete oxidation of benzyl alcohol (>90%) within 3 hours at 80 °C and 3 bar O2 in methanol with a high substrate-to-metal molar ratio of 5800 and turn-over frequency of 0.65 s-1. Factors influencing catalytic activity were investigated, including metal-support interaction, effects of heat treatments, chemical composition of gold clusters, the size of gold nanoparticles and catalytic conditions. It was found that the anions present in gold clusters play a role in determining the catalytic activity in this reaction, with NO3- diminishing the catalytic activity. High catalytic activity was attributed to the formation of large gold nanoparticles (>2 nm) that coincides with partial removal of ligands which occurs during heat treatment and catalysis. Selectivity towards the formation of methyl benzoate can be tuned by selection of the reaction temperature. The catalysts were characterised using transmission electron microscopy, UV-vis diffuse reflectance spectroscopy and X-ray photoelectron spectroscopy.",

author = "Rohul Adnan and Gunther Andersson and Matthew Polson and Gregory Metha and Vladimir Golovko",

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doi = "10.1039/c4cy01168f",

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T1 - Factors influencing the catalytic oxidation of benzyl alcohol using supported phosphine-capped gold nanoparticles

AU - Adnan, Rohul

AU - Andersson, Gunther

AU - Polson, Matthew

AU - Metha, Gregory

AU - Golovko, Vladimir

PY - 2015/2/1

Y1 - 2015/2/1

N2 - Two phosphine-stabilised gold clusters, Au101(PPh3)21Cl5 and Au9(PPh3)8(NO3)3, were deposited and activated on anatase TiO2 and fumed SiO2. These catalysts showed an almost complete oxidation of benzyl alcohol (>90%) within 3 hours at 80 °C and 3 bar O2 in methanol with a high substrate-to-metal molar ratio of 5800 and turn-over frequency of 0.65 s-1. Factors influencing catalytic activity were investigated, including metal-support interaction, effects of heat treatments, chemical composition of gold clusters, the size of gold nanoparticles and catalytic conditions. It was found that the anions present in gold clusters play a role in determining the catalytic activity in this reaction, with NO3- diminishing the catalytic activity. High catalytic activity was attributed to the formation of large gold nanoparticles (>2 nm) that coincides with partial removal of ligands which occurs during heat treatment and catalysis. Selectivity towards the formation of methyl benzoate can be tuned by selection of the reaction temperature. The catalysts were characterised using transmission electron microscopy, UV-vis diffuse reflectance spectroscopy and X-ray photoelectron spectroscopy.

AB - Two phosphine-stabilised gold clusters, Au101(PPh3)21Cl5 and Au9(PPh3)8(NO3)3, were deposited and activated on anatase TiO2 and fumed SiO2. These catalysts showed an almost complete oxidation of benzyl alcohol (>90%) within 3 hours at 80 °C and 3 bar O2 in methanol with a high substrate-to-metal molar ratio of 5800 and turn-over frequency of 0.65 s-1. Factors influencing catalytic activity were investigated, including metal-support interaction, effects of heat treatments, chemical composition of gold clusters, the size of gold nanoparticles and catalytic conditions. It was found that the anions present in gold clusters play a role in determining the catalytic activity in this reaction, with NO3- diminishing the catalytic activity. High catalytic activity was attributed to the formation of large gold nanoparticles (>2 nm) that coincides with partial removal of ligands which occurs during heat treatment and catalysis. Selectivity towards the formation of methyl benzoate can be tuned by selection of the reaction temperature. The catalysts were characterised using transmission electron microscopy, UV-vis diffuse reflectance spectroscopy and X-ray photoelectron spectroscopy.

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JF - Catalysis Science and Technology

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Factors influencing the catalytic oxidation of benzyl alcohol using supported phosphine-capped gold nanoparticles

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