Catalytic oxidative conversion of methane and ethane over polyoxometalate-derived catalysts in electric field at low temperature

Shuhei Ogo; Kousei Iwasaki; Kei Sugiura; Ayaka Sato; Tomohiro Yabe; Yasushi Sekine

doi:10.1016/j.cattod.2017.05.013

Catalytic oxidative conversion of methane and ethane over polyoxometalate-derived catalysts in electric field at low temperature

Shuhei Ogo, Kousei Iwasaki, Kei Sugiura, Ayaka Sato, Tomohiro Yabe, Yasushi Sekine

School of Advanced Science and Engineering

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

14 Citations (Scopus)

Abstract

We examined oxidative coupling of methane (OCM) and oxidative dehydrogenation of ethane (ODE) over various polyoxometalate supported CeO₂ catalysts at 423 K in an electric field. Tetrabutylammonium (TBA) salt of Keggin-type phosphotungstate (PW₁₂O₄₀) supported CeO₂ catalysts ((TBA)₃PW₁₂O₄₀/CeO₂) showed high activities for OCM and ODE in the electric field (3 mA) at 423 K, although the catalyst without the electric field showed extremely low activities at such low temperature. FT-IR spectra and XRD patterns confirmed that the structure of (TBA)₃PW₁₂O₄₀/CeO₂ was changed to Ce₂(WO₄)₃/CeO₂ after reactions with the electric field, and it acted as an active site structure for OCM and ODE with the electric field. Results of activity tests revealed that the C₂H₆ production was a main reaction in OCM with the electric field, and C₂H₄ was formed through a successive oxidative dehydrogenation of the formed C₂H₆. Periodic operation tests demonstrated that reactive oxygen species suitable for ODE were formed on the catalyst surface of Ce₂(WO₄)₃ in the electric field.

Original language	English
Pages (from-to)	80-85
Number of pages	6
Journal	Catalysis Today
Volume	299
DOIs	https://doi.org/10.1016/j.cattod.2017.05.013
Publication status	Published - 2018 Jan 1

Keywords

Cerium tungstate
C–[sbnd]H bond dissociation
Electric field
Ethane oxidative dehydrogenation
Methane oxidative coupling
Polyoxometalate

ASJC Scopus subject areas

Catalysis
Chemistry(all)

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10.1016/j.cattod.2017.05.013

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title = "Catalytic oxidative conversion of methane and ethane over polyoxometalate-derived catalysts in electric field at low temperature",

abstract = "We examined oxidative coupling of methane (OCM) and oxidative dehydrogenation of ethane (ODE) over various polyoxometalate supported CeO2 catalysts at 423 K in an electric field. Tetrabutylammonium (TBA) salt of Keggin-type phosphotungstate (PW12O40) supported CeO2 catalysts ((TBA)3PW12O40/CeO2) showed high activities for OCM and ODE in the electric field (3 mA) at 423 K, although the catalyst without the electric field showed extremely low activities at such low temperature. FT-IR spectra and XRD patterns confirmed that the structure of (TBA)3PW12O40/CeO2 was changed to Ce2(WO4)3/CeO2 after reactions with the electric field, and it acted as an active site structure for OCM and ODE with the electric field. Results of activity tests revealed that the C2H6 production was a main reaction in OCM with the electric field, and C2H4 was formed through a successive oxidative dehydrogenation of the formed C2H6. Periodic operation tests demonstrated that reactive oxygen species suitable for ODE were formed on the catalyst surface of Ce2(WO4)3 in the electric field.",

keywords = "Cerium tungstate, C–[sbnd]H bond dissociation, Electric field, Ethane oxidative dehydrogenation, Methane oxidative coupling, Polyoxometalate",

author = "Shuhei Ogo and Kousei Iwasaki and Kei Sugiura and Ayaka Sato and Tomohiro Yabe and Yasushi Sekine",

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year = "2018",

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T1 - Catalytic oxidative conversion of methane and ethane over polyoxometalate-derived catalysts in electric field at low temperature

AU - Ogo, Shuhei

AU - Iwasaki, Kousei

AU - Sugiura, Kei

AU - Sato, Ayaka

AU - Yabe, Tomohiro

AU - Sekine, Yasushi

PY - 2018/1/1

Y1 - 2018/1/1

N2 - We examined oxidative coupling of methane (OCM) and oxidative dehydrogenation of ethane (ODE) over various polyoxometalate supported CeO2 catalysts at 423 K in an electric field. Tetrabutylammonium (TBA) salt of Keggin-type phosphotungstate (PW12O40) supported CeO2 catalysts ((TBA)3PW12O40/CeO2) showed high activities for OCM and ODE in the electric field (3 mA) at 423 K, although the catalyst without the electric field showed extremely low activities at such low temperature. FT-IR spectra and XRD patterns confirmed that the structure of (TBA)3PW12O40/CeO2 was changed to Ce2(WO4)3/CeO2 after reactions with the electric field, and it acted as an active site structure for OCM and ODE with the electric field. Results of activity tests revealed that the C2H6 production was a main reaction in OCM with the electric field, and C2H4 was formed through a successive oxidative dehydrogenation of the formed C2H6. Periodic operation tests demonstrated that reactive oxygen species suitable for ODE were formed on the catalyst surface of Ce2(WO4)3 in the electric field.

AB - We examined oxidative coupling of methane (OCM) and oxidative dehydrogenation of ethane (ODE) over various polyoxometalate supported CeO2 catalysts at 423 K in an electric field. Tetrabutylammonium (TBA) salt of Keggin-type phosphotungstate (PW12O40) supported CeO2 catalysts ((TBA)3PW12O40/CeO2) showed high activities for OCM and ODE in the electric field (3 mA) at 423 K, although the catalyst without the electric field showed extremely low activities at such low temperature. FT-IR spectra and XRD patterns confirmed that the structure of (TBA)3PW12O40/CeO2 was changed to Ce2(WO4)3/CeO2 after reactions with the electric field, and it acted as an active site structure for OCM and ODE with the electric field. Results of activity tests revealed that the C2H6 production was a main reaction in OCM with the electric field, and C2H4 was formed through a successive oxidative dehydrogenation of the formed C2H6. Periodic operation tests demonstrated that reactive oxygen species suitable for ODE were formed on the catalyst surface of Ce2(WO4)3 in the electric field.

KW - Cerium tungstate

KW - C–[sbnd]H bond dissociation

KW - Electric field

KW - Ethane oxidative dehydrogenation

KW - Methane oxidative coupling

KW - Polyoxometalate

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Catalytic oxidative conversion of methane and ethane over polyoxometalate-derived catalysts in electric field at low temperature

Abstract

Keywords

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