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Reaction mechanism for methane-to-methanol in CU-SSZ-13: First-principles study of the Z 2 [Cu 2 O] and Z 2 [Cu 2 oh] motifs

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Titel: Reaction mechanism for methane-to-methanol in CU-SSZ-13: First-principles study of the Z 2 [Cu 2 O] and Z 2 [Cu 2 oh] motifs
Autoren: Engedahl, Unni, 1990, Arvidsson, Adam, 1990, Grönbeck, Henrik, 1966, Hellman, Anders, 1974
Quelle: Catalysts. 11(1):1-12
Schlagwörter: Copper, Methane-to-methanol, Chabazite, Small-pore zeolite, Direct conversion, DFT, SSZ-13, Reaction mechanism, Micro-kinetic model
Beschreibung: As transportation continues to increase world-wide, there is a need for more efficient utilization of fossil fuel. One possibility is direct conversion of the solution gas bi-product CH4 into an energy-rich, easily usable liquid fuel such as CH3OH. However, new catalytic materials to facilitate the methane-to-methanol reaction are needed. Using density functional calculations, the partial oxidation of methane is investigated over the small-pore copper-exchanged zeolite SSZ-13. The reaction pathway is identified and the energy landscape elucidated over the proposed motifs Z2 [Cu2O] and Z2 [Cu2OH]. It is shown that the Z2[Cu2O] motif has an exergonic reaction path, provided water is added as a solvent for the desorption step. However, a micro-kinetic model shows that neither Z2 [Cu2O] nor Z2 [Cu2OH] has any notable activity under the reaction conditions. These findings highlight the importance of the detailed structure of the active site and that the most stable motif is not necessarily the most active.
Dateibeschreibung: electronic
Zugangs-URL: https://research.chalmers.se/publication/522080
https://research.chalmers.se/publication/522080/file/522080_Fulltext.pdf
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  Data: Reaction mechanism for methane-to-methanol in CU-SSZ-13: First-principles study of the Z 2 [Cu 2 O] and Z 2 [Cu 2 oh] motifs
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  Label: Authors
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  Data: <searchLink fieldCode="AR" term="%22Engedahl%2C+Unni%22">Engedahl, Unni</searchLink>, 1990<br /><searchLink fieldCode="AR" term="%22Arvidsson%2C+Adam%22">Arvidsson, Adam</searchLink>, 1990<br /><searchLink fieldCode="AR" term="%22Grönbeck%2C+Henrik%22">Grönbeck, Henrik</searchLink>, 1966<br /><searchLink fieldCode="AR" term="%22Hellman%2C+Anders%22">Hellman, Anders</searchLink>, 1974
– Name: TitleSource
  Label: Source
  Group: Src
  Data: <i>Catalysts</i>. 11(1):1-12
– Name: Subject
  Label: Subject Terms
  Group: Su
  Data: <searchLink fieldCode="DE" term="%22Copper%22">Copper</searchLink><br /><searchLink fieldCode="DE" term="%22Methane-to-methanol%22">Methane-to-methanol</searchLink><br /><searchLink fieldCode="DE" term="%22Chabazite%22">Chabazite</searchLink><br /><searchLink fieldCode="DE" term="%22Small-pore+zeolite%22">Small-pore zeolite</searchLink><br /><searchLink fieldCode="DE" term="%22Direct+conversion%22">Direct conversion</searchLink><br /><searchLink fieldCode="DE" term="%22DFT%22">DFT</searchLink><br /><searchLink fieldCode="DE" term="%22SSZ-13%22">SSZ-13</searchLink><br /><searchLink fieldCode="DE" term="%22Reaction+mechanism%22">Reaction mechanism</searchLink><br /><searchLink fieldCode="DE" term="%22Micro-kinetic+model%22">Micro-kinetic model</searchLink>
– Name: Abstract
  Label: Description
  Group: Ab
  Data: As transportation continues to increase world-wide, there is a need for more efficient utilization of fossil fuel. One possibility is direct conversion of the solution gas bi-product CH4 into an energy-rich, easily usable liquid fuel such as CH3OH. However, new catalytic materials to facilitate the methane-to-methanol reaction are needed. Using density functional calculations, the partial oxidation of methane is investigated over the small-pore copper-exchanged zeolite SSZ-13. The reaction pathway is identified and the energy landscape elucidated over the proposed motifs Z2 [Cu2O] and Z2 [Cu2OH]. It is shown that the Z2[Cu2O] motif has an exergonic reaction path, provided water is added as a solvent for the desorption step. However, a micro-kinetic model shows that neither Z2 [Cu2O] nor Z2 [Cu2OH] has any notable activity under the reaction conditions. These findings highlight the importance of the detailed structure of the active site and that the most stable motif is not necessarily the most active.
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        Value: 10.3390/catal11010017
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      – Text: English
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        PageCount: 12
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      – SubjectFull: Copper
        Type: general
      – SubjectFull: Methane-to-methanol
        Type: general
      – SubjectFull: Chabazite
        Type: general
      – SubjectFull: Small-pore zeolite
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      – SubjectFull: Direct conversion
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      – SubjectFull: DFT
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      – SubjectFull: SSZ-13
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      – SubjectFull: Reaction mechanism
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      – SubjectFull: Micro-kinetic model
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      – TitleFull: Reaction mechanism for methane-to-methanol in CU-SSZ-13: First-principles study of the Z 2 [Cu 2 O] and Z 2 [Cu 2 oh] motifs
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              Y: 2021
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