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

アクセス数:487件（2025-07-11 08:27 集計）

固定URL: https://hdl.handle.net/11094/98106

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タイトル	Theoretical Investigation of Propylene Epoxidation Using H₂ and O₂ Over Titanosilicate-Supported Au Catalysts
著者	著者名 Hamada, Yasutaka
	著者名 Yonemori, Tomohisa
	著者名 Ishimaru, Yuhki
	NRID 1000030321748 1000030321748 researchmap permalink kawakamitakashi kawakamitakashi Scopus Author ID 7401566433 7401566433 著者名 Kawakami, Takashi
	NRID 1000010324865 1000010324865 researchmap permalink read0068708 read0068708 著者名 Yamanaka, Shusuke
	NRID 1000040356712 1000040356712 researchmap permalink read0118533 read0118533 Scopus Author ID 7203040649 7203040649 著者名 Okumura, Mitsutaka
キーワード等	Au catalysts
	Density functional theory
	Epoxidation of propylene
	Titanosilicate
内容	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.
抄録	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.
出版者	Springer
収録物名	Catalysis Letters
巻(号)	154(11)
ページ	5948-5954
刊行年月	2024-07-30
言語	英語
ハンドルURL	https://hdl.handle.net/11094/98106
PISSN	1011372X
eISSN	1572879X
関連情報 (isIdenticalTo)	DOI (出版社版) https://doi.org/10.1007/s10562-024-04783-y
アクセス権	open access
権利情報	This article is licensed under a Creative Commons Attribution 4.0 International License.
出版タイプ	Version of Record
カテゴリ	学術雑誌論文 Journal Article

資源タイプ	学術雑誌論文
ローカル資源タイプ	学術雑誌論文
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	英語
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	英語
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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