Theoretical Investigation of Propylene Epoxidation Using H₂ and O₂ Over Titanosilicate-Supported Au Catalysts

Hamada, Yasutaka; Yonemori, Tomohisa; Ishimaru, Yuhki; Kawakami, Takashi; Yamanaka, Shusuke; Okumura, Mitsutaka

doi:https://doi.org/10.1007/s10562-024-04783-y

Theoretical Investigation of Propylene Epoxidation Using H₂ and O₂ Over Titanosilicate-Supported Au Catalysts

Hamada, Yasutaka; Yonemori, Tomohisa; Ishimaru, Yuhki et al.

Catalysis Letters, 2024, 154(11), 5948-5954

Number of Access:535（2025-08-14 02:42 Counts）

Identifier to cite or link to this item: https://hdl.handle.net/11094/98106

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Title	Theoretical Investigation of Propylene Epoxidation Using H₂ and O₂ Over Titanosilicate-Supported Au Catalysts
Creator	CreatorName Hamada, Yasutaka
	CreatorName Yonemori, Tomohisa
	CreatorName Ishimaru, Yuhki
	NRID 1000030321748 1000030321748 researchmap permalink kawakamitakashi kawakamitakashi Scopus Author ID 7401566433 7401566433 CreatorName Kawakami, Takashi
	NRID 1000010324865 1000010324865 researchmap permalink read0068708 read0068708 CreatorName Yamanaka, Shusuke
	NRID 1000040356712 1000040356712 researchmap permalink read0118533 read0118533 Scopus Author ID 7203040649 7203040649 CreatorName Okumura, Mitsutaka
Subject	Au catalysts
	Density functional theory
	Epoxidation of propylene
	Titanosilicate
Description	The version of record of this article, first published in Catalysis Letters, is available online at Publisher’s website: https://doi.org/10.1007/s10562-024-04783-y.
Abstract	Titanosilicate-supported Au-cluster catalysts can be used to selectively synthesize propylene oxide from propylene using O₂ and H₂. However, the details of the catalytic reaction mechanism have not yet been elucidated. Thus, the reaction mechanism was investigated using density functional theory calculations. The calculation results revealed that active Ti-OOH forms on the surface Ti site, which is active as an oxidant and acts as an anchorage site for Au nanoclusters. The rate-determining step of propylene oxide synthesis on Au/titanosilicate is O insertion into propylene, with an activation energy of 1.37 eV. The propylene involved in this reaction is activated by adsorption on Au nanoclusters. Moreover, it was also found that the formation of Ti-OOH on Au/titanosilicate requires an activation energy of 0.48 eV, while it is barrierless on Au/anatase-TiO₂. However, the decomposition energy of Ti-OOH on Au/titanosilicate is −0.16 eV, which is smaller than that on Au/anatase-TiO₂ (−1.12 eV). The results indicate that Ti-OOH decomposes more readily on Au/titanosilicate than on Au/anatase-TiO₂ but is easily regenerated because the reaction energy is significantly smaller than that on Au/anatase-TiO₂. Therefore, these calculations are qualitatively in good agreement with the experimental results for Au/titanosilicate, which exhibited high catalytic activity at high temperatures.
Publisher	Springer
Source Title	Catalysis Letters
Volume (Issue)	154(11)
Page	5948-5954
Date of Issued	2024-07-30
Language	English
Handle URL	https://hdl.handle.net/11094/98106
PISSN	1011372X
eISSN	1572879X
Relation.isIdenticalTo	DOI (Publisher Version) https://doi.org/10.1007/s10562-024-04783-y
Access Rights	open access
CopyRight	This article is licensed under a Creative Commons Attribution 4.0 International License.
oaire:version	Version of Record
Category	学術雑誌論文 Journal Article

Resource Type	journal article
Local Type	Journal Article
DCTERMS.bibliographicCitation	Catalysis Letters. 2024, 154(11), p. 5948-5954
DC.title	Theoretical Investigation of Propylene Epoxidation Using H₂ and O₂ Over Titanosilicate-Supported Au Catalysts
DC.creator	Hamada, Yasutaka
	Yonemori, Tomohisa
	Ishimaru, Yuhki
	Kawakami, Takashi
	Yamanaka, Shusuke
	Okumura, Mitsutaka
DC.publisher	Springer
DC.language' scheme='DCTERMS.RFC1766	English
DCTERMS.issued' scheme='DCTERMS.W3CDTF	2024-07-30
DC.identifier	https://doi.org/10.1007/s10562-024-04783-y
DC.subject	Au catalysts
	Density functional theory
	Epoxidation of propylene
	Titanosilicate
DC.description	The version of record of this article, first published in Catalysis Letters, is available online at Publisher’s website: https://doi.org/10.1007/s10562-024-04783-y.
DCTERMS.abstract	Titanosilicate-supported Au-cluster catalysts can be used to selectively synthesize propylene oxide from propylene using O₂ and H₂. However, the details of the catalytic reaction mechanism have not yet been elucidated. Thus, the reaction mechanism was investigated using density functional theory calculations. The calculation results revealed that active Ti-OOH forms on the surface Ti site, which is active as an oxidant and acts as an anchorage site for Au nanoclusters. The rate-determining step of propylene oxide synthesis on Au/titanosilicate is O insertion into propylene, with an activation energy of 1.37 eV. The propylene involved in this reaction is activated by adsorption on Au nanoclusters. Moreover, it was also found that the formation of Ti-OOH on Au/titanosilicate requires an activation energy of 0.48 eV, while it is barrierless on Au/anatase-TiO₂. However, the decomposition energy of Ti-OOH on Au/titanosilicate is −0.16 eV, which is smaller than that on Au/anatase-TiO₂ (−1.12 eV). The results indicate that Ti-OOH decomposes more readily on Au/titanosilicate than on Au/anatase-TiO₂ but is easily regenerated because the reaction energy is significantly smaller than that on Au/anatase-TiO₂. Therefore, these calculations are qualitatively in good agreement with the experimental results for Au/titanosilicate, which exhibited high catalytic activity at high temperatures.
DC.rights	This article is licensed under a Creative Commons Attribution 4.0 International License.
DC.format	98106
citation_title	Theoretical Investigation of Propylene Epoxidation Using H₂ and O₂ Over Titanosilicate-Supported Au Catalysts
citation_author	Hamada, Yasutaka
	Yonemori, Tomohisa
	Ishimaru, Yuhki
	Kawakami, Takashi
	Yamanaka, Shusuke
	Okumura, Mitsutaka
citation_publisher	Springer
citation_language	English
citation_date	2024-07-30
citation_journal_title	Catalysis Letters
citation_volume	154
citation_issue	11
citation_firstpage	5948
citation_lastpage	5954
citation_doi	https://doi.org/10.1007/s10562-024-04783-y
citation_public_url	https://hdl.handle.net/11094/98106

Theoretical Investigation of Propylene Epoxidation Using H₂ and O₂ Over Titanosilicate-Supported Au Catalysts

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