A MAS NMR and DRIFT study of the Ga species in Ga/H-ZSM5 catalysts and their effect on propane ammoxidation

P. Pal; J. Quartararo; S.B. Hamid, abd; E.G. Derouane; J.C. Védrine; P.C.M.M. Magusin; B.G. Anderson

doi:10.1139/v05-073

A MAS NMR and DRIFT study of the Ga species in Ga/H-ZSM5 catalysts and their effect on propane ammoxidation

P. Pal, J. Quartararo, S.B. Hamid, abd, E.G. Derouane, J.C. Védrine, P.C.M.M. Magusin, B.G. Anderson

Inorganic Materials & Catalysis

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Abstract

71Ga, 27Al and 29Si MAS-NMR and DRIFT spectroscopies were used to characterize the state of gallium in Ga/H-ZSM5 catalysts tested for their ability to catalyse the ammoxidation of propane. Ga-species were observed in two different possible environments: octahedrally-coordinated gallium in small Ga2O3 particles at the external surface of the zeolite crystals, octahedrally-coordinated gallium in GaO(OH) or related species, and tetrahedrally-coordinated gallium in cationic-exchange positions inside the zeolite. Redox (H2-O2) cycles promote the migration of gallium from the GaO(OH) or Ga2O3 species at the external surface of the zeolite crystals to cationic-exchange sites within the zeolite channels. The redox treatment definitely had a beneficial effect on its catalytic performance for the ammoxidation of propane, which is known to occur via a bifunctional mechanism. The main product was acetonitrile at high Ga and Al contents while acrylonitrile was also observed as a side product at high Ga and low Al contents.

Original language	English
Pages (from-to)	574-580
Journal	Canadian Journal of Chemistry
Volume	83
Issue number	6-7
DOIs	https://doi.org/10.1139/v05-073
Publication status	Published - 2005

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@article{9bd1db8f7a3344318124d212698d67af,

title = "A MAS NMR and DRIFT study of the Ga species in Ga/H-ZSM5 catalysts and their effect on propane ammoxidation",

abstract = "71Ga, 27Al and 29Si MAS-NMR and DRIFT spectroscopies were used to characterize the state of gallium in Ga/H-ZSM5 catalysts tested for their ability to catalyse the ammoxidation of propane. Ga-species were observed in two different possible environments: octahedrally-coordinated gallium in small Ga2O3 particles at the external surface of the zeolite crystals, octahedrally-coordinated gallium in GaO(OH) or related species, and tetrahedrally-coordinated gallium in cationic-exchange positions inside the zeolite. Redox (H2-O2) cycles promote the migration of gallium from the GaO(OH) or Ga2O3 species at the external surface of the zeolite crystals to cationic-exchange sites within the zeolite channels. The redox treatment definitely had a beneficial effect on its catalytic performance for the ammoxidation of propane, which is known to occur via a bifunctional mechanism. The main product was acetonitrile at high Ga and Al contents while acrylonitrile was also observed as a side product at high Ga and low Al contents.",

author = "P. Pal and J. Quartararo and {Hamid, abd}, S.B. and E.G. Derouane and J.C. V{\'e}drine and P.C.M.M. Magusin and B.G. Anderson",

year = "2005",

doi = "10.1139/v05-073",

language = "English",

volume = "83",

pages = "574--580",

journal = "Canadian Journal of Chemistry",

issn = "0008-4042",

publisher = "National Research Council of Canada",

number = "6-7",

}

TY - JOUR

T1 - A MAS NMR and DRIFT study of the Ga species in Ga/H-ZSM5 catalysts and their effect on propane ammoxidation

AU - Pal, P.

AU - Quartararo, J.

AU - Hamid, abd, S.B.

AU - Derouane, E.G.

AU - Védrine, J.C.

AU - Magusin, P.C.M.M.

AU - Anderson, B.G.

PY - 2005

Y1 - 2005

N2 - 71Ga, 27Al and 29Si MAS-NMR and DRIFT spectroscopies were used to characterize the state of gallium in Ga/H-ZSM5 catalysts tested for their ability to catalyse the ammoxidation of propane. Ga-species were observed in two different possible environments: octahedrally-coordinated gallium in small Ga2O3 particles at the external surface of the zeolite crystals, octahedrally-coordinated gallium in GaO(OH) or related species, and tetrahedrally-coordinated gallium in cationic-exchange positions inside the zeolite. Redox (H2-O2) cycles promote the migration of gallium from the GaO(OH) or Ga2O3 species at the external surface of the zeolite crystals to cationic-exchange sites within the zeolite channels. The redox treatment definitely had a beneficial effect on its catalytic performance for the ammoxidation of propane, which is known to occur via a bifunctional mechanism. The main product was acetonitrile at high Ga and Al contents while acrylonitrile was also observed as a side product at high Ga and low Al contents.

AB - 71Ga, 27Al and 29Si MAS-NMR and DRIFT spectroscopies were used to characterize the state of gallium in Ga/H-ZSM5 catalysts tested for their ability to catalyse the ammoxidation of propane. Ga-species were observed in two different possible environments: octahedrally-coordinated gallium in small Ga2O3 particles at the external surface of the zeolite crystals, octahedrally-coordinated gallium in GaO(OH) or related species, and tetrahedrally-coordinated gallium in cationic-exchange positions inside the zeolite. Redox (H2-O2) cycles promote the migration of gallium from the GaO(OH) or Ga2O3 species at the external surface of the zeolite crystals to cationic-exchange sites within the zeolite channels. The redox treatment definitely had a beneficial effect on its catalytic performance for the ammoxidation of propane, which is known to occur via a bifunctional mechanism. The main product was acetonitrile at high Ga and Al contents while acrylonitrile was also observed as a side product at high Ga and low Al contents.

U2 - 10.1139/v05-073

DO - 10.1139/v05-073

M3 - Article

SN - 0008-4042

VL - 83

SP - 574

EP - 580

JO - Canadian Journal of Chemistry

JF - Canadian Journal of Chemistry

IS - 6-7

ER -

A MAS NMR and DRIFT study of the Ga species in Ga/H-ZSM5 catalysts and their effect on propane ammoxidation

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