Structure-reactivity correlations in sulphated-zirconia catalysts for the isomerisation of α-pinene

Muriel A. Ecormier; Karen Wilson; Adam F. Lee

doi:10.1016/S0021-9517(02)00150-1

Structure-reactivity correlations in sulphated-zirconia catalysts for the isomerisation of α-pinene

Muriel A. Ecormier, Karen Wilson, Adam F. Lee

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

Abstract

A range of mesoporous sulphated zirconias with tuneable structural and catalytic properties have been prepared by direct impregnation. The surface sulphate coverage can be readily varied, achieving a maximum value of ∼0.2 monolayers. High-temperature calcination induces the crystallisation of tetragonal zirconia while suppressing the monoclinic phase and enhances surface acidity. Superacid sites only appear above a critical threshold SO₄ coverage of 0.08 mL (corresponding to 0.44 wt% total S). Sulphated zirconias show good activity towards α-pinene isomerisation of under mild conditions. Conversion correlates with the number Brønsted acid sites, while the selectivity towards mono- versus polycyclic products depends on the corresponding acid site strength; superacidity promotes limonene formation over camphene.

Original language	English
Pages (from-to)	57-65
Number of pages	9
Journal	Journal of Catalysis
Volume	215
Issue number	1
Early online date	19 Mar 2003
DOIs	https://doi.org/10.1016/S0021-9517(02)00150-1
Publication status	Published - 1 Apr 2003

Keywords

solid acid catalysts
clean technology
green chemistry
zirconia
α-pinene

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10.1016/S0021-9517(02)00150-1

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AU - Wilson, Karen

AU - Lee, Adam F.

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N2 - A range of mesoporous sulphated zirconias with tuneable structural and catalytic properties have been prepared by direct impregnation. The surface sulphate coverage can be readily varied, achieving a maximum value of ∼0.2 monolayers. High-temperature calcination induces the crystallisation of tetragonal zirconia while suppressing the monoclinic phase and enhances surface acidity. Superacid sites only appear above a critical threshold SO4 coverage of 0.08 mL (corresponding to 0.44 wt% total S). Sulphated zirconias show good activity towards α-pinene isomerisation of under mild conditions. Conversion correlates with the number Brønsted acid sites, while the selectivity towards mono- versus polycyclic products depends on the corresponding acid site strength; superacidity promotes limonene formation over camphene.

AB - A range of mesoporous sulphated zirconias with tuneable structural and catalytic properties have been prepared by direct impregnation. The surface sulphate coverage can be readily varied, achieving a maximum value of ∼0.2 monolayers. High-temperature calcination induces the crystallisation of tetragonal zirconia while suppressing the monoclinic phase and enhances surface acidity. Superacid sites only appear above a critical threshold SO4 coverage of 0.08 mL (corresponding to 0.44 wt% total S). Sulphated zirconias show good activity towards α-pinene isomerisation of under mild conditions. Conversion correlates with the number Brønsted acid sites, while the selectivity towards mono- versus polycyclic products depends on the corresponding acid site strength; superacidity promotes limonene formation over camphene.

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KW - clean technology

KW - green chemistry

KW - zirconia

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Structure-reactivity correlations in sulphated-zirconia catalysts for the isomerisation of α-pinene

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