Dehydration mechanism of ethanol in the pseudoliquid phase of H3-xCsxPW12O40

Toshio Okuhara; Takeo Arai; Tatsumi Ichiki; Kwan Young Lee; Makato Misono

doi:10.1016/0304-5102(89)80263-9

Dehydration mechanism of ethanol in the pseudoliquid phase of H_3-xCs_xPW₁₂O₄₀

Toshio Okuhara, Takeo Arai, Tatsumi Ichiki, Kwan Young Lee, Makato Misono

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

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Abstract

Dehydration of ethanol catalyzed by H_3-xCs_xPW₁₂O₄₀ has been studied by a transient response method and solid-state NMR spectroscopy. An unusual pressure dependency was observed for catalysts with x ≤ 2. This has been explained by assuming (1) that C₂H₅OH⁺₂ and (C₂H₅OH)₂H⁺ act as intermediates for the formation of ethylene and ether, respectively, in the pseudoliquid phase and (2) that the concentrations of these intermediates are determined by protonation equilibria established in the system. The presence of these species as well as of an ethoxy group has been detected directly by solid-state NMR spectroscopy in the case of H₃PW₁₂O₄₀. Dehydration over H_0.5Cs_2.5PW₁₂O₄₀ proceeded by surface reaction as in the case of ordinary acid solids.

Original language	English
Pages (from-to)	293-301
Number of pages	9
Journal	Journal of Molecular Catalysis
Volume	55
Issue number	1
DOIs	https://doi.org/10.1016/0304-5102(89)80263-9
Publication status	Published - 1989 Nov 1
Externally published	Yes

ASJC Scopus subject areas

Engineering(all)

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10.1016/0304-5102(89)80263-9

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title = "Dehydration mechanism of ethanol in the pseudoliquid phase of H3-xCsxPW12O40",

abstract = "Dehydration of ethanol catalyzed by H3-xCsxPW12O40 has been studied by a transient response method and solid-state NMR spectroscopy. An unusual pressure dependency was observed for catalysts with x ≤ 2. This has been explained by assuming (1) that C2H5OH+2 and (C2H5OH)2H+ act as intermediates for the formation of ethylene and ether, respectively, in the pseudoliquid phase and (2) that the concentrations of these intermediates are determined by protonation equilibria established in the system. The presence of these species as well as of an ethoxy group has been detected directly by solid-state NMR spectroscopy in the case of H3PW12O40. Dehydration over H0.5Cs2.5PW12O40 proceeded by surface reaction as in the case of ordinary acid solids.",

author = "Toshio Okuhara and Takeo Arai and Tatsumi Ichiki and Lee, {Kwan Young} and Makato Misono",

note = "Funding Information: The authors would like to thank Drs Shin-ichi Nakata and Sachio Asaoka (Chiyoda Chemical Engineering & Construction Co. Ltd.) for the solid-state NMR measurements and helpful discussions. This study was supported by Grant-in-Aid for Scientific Research No. 62 470 070 from the Ministry of Education, Science and Culture of Japan.",

year = "1989",

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doi = "10.1016/0304-5102(89)80263-9",

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T1 - Dehydration mechanism of ethanol in the pseudoliquid phase of H3-xCsxPW12O40

AU - Okuhara, Toshio

AU - Arai, Takeo

AU - Ichiki, Tatsumi

AU - Lee, Kwan Young

AU - Misono, Makato

N1 - Funding Information: The authors would like to thank Drs Shin-ichi Nakata and Sachio Asaoka (Chiyoda Chemical Engineering & Construction Co. Ltd.) for the solid-state NMR measurements and helpful discussions. This study was supported by Grant-in-Aid for Scientific Research No. 62 470 070 from the Ministry of Education, Science and Culture of Japan.

PY - 1989/11/1

Y1 - 1989/11/1

N2 - Dehydration of ethanol catalyzed by H3-xCsxPW12O40 has been studied by a transient response method and solid-state NMR spectroscopy. An unusual pressure dependency was observed for catalysts with x ≤ 2. This has been explained by assuming (1) that C2H5OH+2 and (C2H5OH)2H+ act as intermediates for the formation of ethylene and ether, respectively, in the pseudoliquid phase and (2) that the concentrations of these intermediates are determined by protonation equilibria established in the system. The presence of these species as well as of an ethoxy group has been detected directly by solid-state NMR spectroscopy in the case of H3PW12O40. Dehydration over H0.5Cs2.5PW12O40 proceeded by surface reaction as in the case of ordinary acid solids.

AB - Dehydration of ethanol catalyzed by H3-xCsxPW12O40 has been studied by a transient response method and solid-state NMR spectroscopy. An unusual pressure dependency was observed for catalysts with x ≤ 2. This has been explained by assuming (1) that C2H5OH+2 and (C2H5OH)2H+ act as intermediates for the formation of ethylene and ether, respectively, in the pseudoliquid phase and (2) that the concentrations of these intermediates are determined by protonation equilibria established in the system. The presence of these species as well as of an ethoxy group has been detected directly by solid-state NMR spectroscopy in the case of H3PW12O40. Dehydration over H0.5Cs2.5PW12O40 proceeded by surface reaction as in the case of ordinary acid solids.

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Dehydration mechanism of ethanol in the pseudoliquid phase of H_3-xCs_xPW₁₂O₄₀

Abstract

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