Selective production of hydrogen isotope gases via PdAg-catalyzed dehydrogenation of formic acid in D2O assisted by surface-grafted amine groups

Mori, Kohsuke; Konishi, Atsushi; Fujita, Tatsuya; Yamashita, Hiromi

doi:https://doi.org/10.1016/j.mtsust.2023.100407

Selective production of hydrogen isotope gases via PdAg-catalyzed dehydrogenation of formic acid in D2O assisted by surface-grafted amine groups

Mori, Kohsuke; Konishi, Atsushi; Fujita, Tatsuya et al.

Materials Today Sustainability, 2023, 22, 100407

アクセス数:422件（2025-10-09 04:15 集計）

固定URL: https://hdl.handle.net/11094/94006

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タイトル	Selective production of hydrogen isotope gases via PdAg-catalyzed dehydrogenation of formic acid in D2O assisted by surface-grafted amine groups
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 Konishi, Atsushi
	著者名 Fujita, Tatsuya
	NRID 1000040200688 1000040200688 researchmap permalink read0118536 read0118536 Scopus Author ID 7403649198 7403649198 著者名 Yamashita, Hiromi
キーワード等	Alloy nanoparticles
	Amine modification
	Deuterium gas
	Hydrogen deuteride
内容	Mori K., Konishi A., Fujita T., et al. Selective production of hydrogen isotope gases via PdAg-catalyzed dehydrogenation of formic acid in D2O assisted by surface-grafted amine groups. Materials Today Sustainability 22, 100407 (2023); https://doi.org/10.1016/j.mtsust.2023.100407.
抄録	Hydrogen isotope gases are widely used as deuterium sources in industrial manufacturing processes. It would therefore be beneficial to develop a facile, simple means of selective producing molecular deuterium (D2) and hydrogen deuteride (HD), although reasonable heterogeneous catalytic methodologies are still missing. We previously demonstrated that the hydrogen isotope gases was selectively obtained from formic acid (HCOOH, FA) and D2O using PdAg nanoparticles supported on mesoporous silica (SBA-15) on which amine functional groups had been grafted. In the present work, amine-functionalized carbon was used as an efficient support material to provide a catalyst with improved activity. Employing weakly basic phenylamine groups, D2 was predominantly evolved and the reaction rate was doubled compared with that for our previously reported system. A high degree of correlation between D2 selectivity and the basicity of the grafted amine groups was also observed. The applicability of the present catalytic system was highlighted by in situ deuteration of diphenylacetylene in a solution of FA in D2O, during which deuterated products were obtained with high efficiency.
出版者	Elsevier Ltd
収録物名	Materials Today Sustainability
巻(号)	22
ページ	100407
刊行年月	2023-06-01
言語	英語
ハンドルURL	https://hdl.handle.net/11094/94006
eISSN	25892347
関連情報 (isVersionOf)	DOI (出版社版) https://doi.org/10.1016/j.mtsust.2023.100407
アクセス権	open access
権利情報	© 2023. This manuscript version is made available under the CC-BY-NC-ND 4.0 license https://creativecommons.org/licenses/by-nc-nd/4.0/
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
DCMI資源タイプ	text
DCTERMS.bibliographicCitation	Materials Today Sustainability. 2023, 22, p. 100407
DC.title	Selective production of hydrogen isotope gases via PdAg-catalyzed dehydrogenation of formic acid in D2O assisted by surface-grafted amine groups
DC.creator	Mori, Kohsuke
	Konishi, Atsushi
	Fujita, Tatsuya
	Yamashita, Hiromi
DC.publisher	Elsevier Ltd
DC.language' scheme='DCTERMS.RFC1766	英語
DC.type' scheme='DCTERMS.DCMIType	text
DCTERMS.issued' scheme='DCTERMS.W3CDTF	2023-06-01
DC.identifier	https://doi.org/10.1016/j.mtsust.2023.100407
DC.subject	Alloy nanoparticles
	Amine modification
	Deuterium gas
	Hydrogen deuteride
DC.description	Mori K., Konishi A., Fujita T., et al. Selective production of hydrogen isotope gases via PdAg-catalyzed dehydrogenation of formic acid in D2O assisted by surface-grafted amine groups. Materials Today Sustainability 22, 100407 (2023); https://doi.org/10.1016/j.mtsust.2023.100407.
DCTERMS.abstract	Hydrogen isotope gases are widely used as deuterium sources in industrial manufacturing processes. It would therefore be beneficial to develop a facile, simple means of selective producing molecular deuterium (D2) and hydrogen deuteride (HD), although reasonable heterogeneous catalytic methodologies are still missing. We previously demonstrated that the hydrogen isotope gases was selectively obtained from formic acid (HCOOH, FA) and D2O using PdAg nanoparticles supported on mesoporous silica (SBA-15) on which amine functional groups had been grafted. In the present work, amine-functionalized carbon was used as an efficient support material to provide a catalyst with improved activity. Employing weakly basic phenylamine groups, D2 was predominantly evolved and the reaction rate was doubled compared with that for our previously reported system. A high degree of correlation between D2 selectivity and the basicity of the grafted amine groups was also observed. The applicability of the present catalytic system was highlighted by in situ deuteration of diphenylacetylene in a solution of FA in D2O, during which deuterated products were obtained with high efficiency.
DC.rights	© 2023. This manuscript version is made available under the CC-BY-NC-ND 4.0 license https://creativecommons.org/licenses/by-nc-nd/4.0/
DC.format	94006
citation_title	Selective production of hydrogen isotope gases via PdAg-catalyzed dehydrogenation of formic acid in D2O assisted by surface-grafted amine groups
citation_author	Mori, Kohsuke
	Konishi, Atsushi
	Fujita, Tatsuya
	Yamashita, Hiromi
citation_publisher	Elsevier Ltd
citation_language	英語
citation_date	2023-06-01
citation_journal_title	Materials Today Sustainability
citation_volume	22
citation_firstpage	100407
citation_doi	https://doi.org/10.1016/j.mtsust.2023.100407
citation_public_url	https://hdl.handle.net/11094/94006

Selective production of hydrogen isotope gases via PdAg-catalyzed dehydrogenation of formic acid in D2O assisted by surface-grafted amine groups

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