Entropy-Stabilized Isolated Active Pd Species within a High-Entropy Fluorite Oxide Matrix for CO₂ Hydrogenation to Formic Acid

Mori, Kohsuke; Shimada, Yuki; Yoshida, Hideto; Yamashita, Hiromi

doi:https://doi.org/10.1021/acsanm.4c05908

Entropy-Stabilized Isolated Active Pd Species within a High-Entropy Fluorite Oxide Matrix for CO₂ Hydrogenation to Formic Acid

Mori, Kohsuke; Shimada, Yuki; Yoshida, Hideto et al.

ACS Applied Nano Materials, 2024, 7(24), 28649-28658

アクセス数:820件（2026-02-16 09:47 集計）

固定URL: https://hdl.handle.net/11094/100147

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タイトル	Entropy-Stabilized Isolated Active Pd Species within a High-Entropy Fluorite Oxide Matrix for CO₂ Hydrogenation to Formic Acid
著者	NRID 1000090423087 1000090423087 ORCID 0000-0003-3915-4528 0000-0003-3915-4528 researchmap permalink 7000018582 7000018582 Scopus Author ID 35426128700 35426128700 著者名 Mori, Kohsuke
	著者名 Shimada, Yuki
	NRID 1000000452425 1000000452425 ORCID 0000-0002-4195-3225 0000-0002-4195-3225 researchmap permalink read0204918 read0204918 Scopus Author ID 55324307600 55324307600 著者名 Yoshida, Hideto
	NRID 1000040200688 1000040200688 researchmap permalink read0118536 read0118536 Scopus Author ID 7403649198 7403649198 著者名 Yamashita, Hiromi
キーワード等	high-entropy oxides
	palladium
	catalyst
	formic acid
	carbon dioxide
内容	Mori K., Shimada Y., Yoshida H., et al. Entropy-Stabilized Isolated Active Pd Species within a High-Entropy Fluorite Oxide Matrix for CO₂ Hydrogenation to Formic Acid. ACS Applied Nano Materials 7, 28649 (2024); https://doi.org/10.1021/acsanm.4c05908.
抄録	Active, stable Pd species were incorporated within the matrix of fluorite-based high-entropy oxide (HEO) (YZrLaGdHf)xO2 using an entropy-driven strategy based on a liquid-phase reaction. In situ X-ray absorption fine structure analyses and transmission electron microscopy observations at elevated temperatures under H2 confirmed that partially aggregated Pd oxide species in the as-synthesized Pd@(YZrLaGdHf)xO2 were transformed into an entropy-stabilized isolated form at 600 °C. In contrast, Pd species on the (YZrLaGdHf)xO2 surface were readily reduced with the formation of nanoclusters/nanoparticles even in the temperature range of 100 to 200 °C. This Pd@(YZrLaGdHf)xO2 exhibited enhanced activity during the hydrogenation of CO2 to formic acid with a maximum turnover number of 5000 based on the quantity of surface-exposed Pd atoms. This performance was more than eight times higher than that of the Pd/(YZrLaGdHf)xO2 on the basis of supported Pd. An assessment of the kinetics and theoretical investigations suggested that entropy-stabilized isolated Pd species facilitated both H2 dissociation and the attack of dissociated H atoms on C atoms in HCO3– ions.
出版者	American Chemical Society
収録物名	ACS Applied Nano Materials
巻(号)	7(24)
ページ	28649-28658
刊行年月	2024-12-27
言語	英語
ハンドルURL	https://hdl.handle.net/11094/100147
eISSN	25740970
関連情報 (isVersionOf)	DOI (出版社版) https://doi.org/10.1021/acsanm.4c05908
アクセス権	open access
権利情報	This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Applied Nano Materials, © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acsanm.4c05908.
出版タイプ	Accepted Manuscript
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	ACS Applied Nano Materials. 2024, 7(24), p. 28649-28658
DC.title	Entropy-Stabilized Isolated Active Pd Species within a High-Entropy Fluorite Oxide Matrix for CO₂ Hydrogenation to Formic Acid
DC.creator	Mori, Kohsuke
	Shimada, Yuki
	Yoshida, Hideto
	Yamashita, Hiromi
DC.publisher	American Chemical Society
DC.language' scheme='DCTERMS.RFC1766	英語
DCTERMS.issued' scheme='DCTERMS.W3CDTF	2024-12-27
DC.identifier	https://doi.org/10.1021/acsanm.4c05908
DC.subject	high-entropy oxides
	palladium
	catalyst
	formic acid
	carbon dioxide
DC.description	Mori K., Shimada Y., Yoshida H., et al. Entropy-Stabilized Isolated Active Pd Species within a High-Entropy Fluorite Oxide Matrix for CO₂ Hydrogenation to Formic Acid. ACS Applied Nano Materials 7, 28649 (2024); https://doi.org/10.1021/acsanm.4c05908.
DCTERMS.abstract	Active, stable Pd species were incorporated within the matrix of fluorite-based high-entropy oxide (HEO) (YZrLaGdHf)xO2 using an entropy-driven strategy based on a liquid-phase reaction. In situ X-ray absorption fine structure analyses and transmission electron microscopy observations at elevated temperatures under H2 confirmed that partially aggregated Pd oxide species in the as-synthesized Pd@(YZrLaGdHf)xO2 were transformed into an entropy-stabilized isolated form at 600 °C. In contrast, Pd species on the (YZrLaGdHf)xO2 surface were readily reduced with the formation of nanoclusters/nanoparticles even in the temperature range of 100 to 200 °C. This Pd@(YZrLaGdHf)xO2 exhibited enhanced activity during the hydrogenation of CO2 to formic acid with a maximum turnover number of 5000 based on the quantity of surface-exposed Pd atoms. This performance was more than eight times higher than that of the Pd/(YZrLaGdHf)xO2 on the basis of supported Pd. An assessment of the kinetics and theoretical investigations suggested that entropy-stabilized isolated Pd species facilitated both H2 dissociation and the attack of dissociated H atoms on C atoms in HCO3– ions.
DC.rights	This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Applied Nano Materials, © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acsanm.4c05908.
DC.format	100147
citation_title	Entropy-Stabilized Isolated Active Pd Species within a High-Entropy Fluorite Oxide Matrix for CO₂ Hydrogenation to Formic Acid
citation_author	Mori, Kohsuke
	Shimada, Yuki
	Yoshida, Hideto
	Yamashita, Hiromi
citation_publisher	American Chemical Society
citation_language	英語
citation_date	2024-12-27
citation_journal_title	ACS Applied Nano Materials
citation_volume	7
citation_issue	24
citation_firstpage	28649
citation_lastpage	28658
citation_doi	https://doi.org/10.1021/acsanm.4c05908
citation_public_url	https://hdl.handle.net/11094/100147

Entropy-Stabilized Isolated Active Pd Species within a High-Entropy Fluorite Oxide Matrix for CO₂ Hydrogenation to Formic Acid

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