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[Fe4] and [Fe6] Hydride Clusters Supported by Phosphines: Synthesis, Characterization, and Application in N2 Reduction
http://hdl.handle.net/2237/26770
http://hdl.handle.net/2237/267705dc8b6fb-03db-418d-bbae-3eb42258904e
名前 / ファイル | ライセンス | アクション |
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Fe-hydride_rev-manuscript.pdf ファイル公開:2018/04/19 (2.0 MB)
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Item type | 学術雑誌論文 / Journal Article(1) | |||||
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公開日 | 2017-07-05 | |||||
タイトル | ||||||
タイトル | [Fe4] and [Fe6] Hydride Clusters Supported by Phosphines: Synthesis, Characterization, and Application in N2 Reduction | |||||
言語 | en | |||||
著者 |
Araake, Ryoichi
× Araake, Ryoichi× Sakadani, Kazuki× Tada, Mizuki× Sakai, Yoichi× Ohki, Yasuhiro |
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アクセス権 | ||||||
アクセス権 | open access | |||||
アクセス権URI | http://purl.org/coar/access_right/c_abf2 | |||||
権利 | ||||||
言語 | en | |||||
権利情報 | “This document is the Accepted Manuscript version of a Published Work that appeared in final form in [Journal of the American Chemical Society], copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see [http://pubs.acs.org/articlesonrequest/AOR-K5XfZzY9fyF5yEGKJc3j].” | |||||
抄録 | ||||||
内容記述 | Multiple iron atoms bridged by hydrides is a common structural feature of the active species that have been postulated in the biological and industrial reduction of N2. In this study, the reactions of an Fe(II) amide complex with pinacolborane in the presence/absence of phosphines afforded a series of hydride-supported [Fe4] and [Fe6] clusters Fe4(μ-H)4(μ3-H)2{N(SiMe3)2}2(PR3)4 (PR3 = PMe3 (2a), PMe2Ph (2b), PEt3 (2c)), Fe6(μ-H)10(μ3-H)2(PMe3)10 (3), and (η6-C7H8)Fe4(μ-H)2{μ-N(SiMe3)2}2{N(SiMe3)2}2 (4), which were characterized crystallographically and spectroscopically. Under ambient conditions, these clusters catalyzed the silylation of N2 to furnish up to 160 ± 13 equiv of N(SiMe3)3 per 2c (40 equiv per Fe atom) and 183 ± 18 equiv per 3 (31 equiv per Fe atom). With regard to the generation of the reactive species, dissociation of phosphine and hydride ligands from the [Fe4] and [Fe6] clusters was indicated, based on the results of the mass spectrometric analysis on the [Fe6] cluster, as well as the formation of a diphenylsilane adduct of the [Fe4] cluster. | |||||
言語 | en | |||||
内容記述タイプ | Abstract | |||||
出版者 | ||||||
言語 | en | |||||
出版者 | ACS Publications | |||||
言語 | ||||||
言語 | eng | |||||
資源タイプ | ||||||
資源タイプresource | http://purl.org/coar/resource_type/c_6501 | |||||
タイプ | journal article | |||||
出版タイプ | ||||||
出版タイプ | AM | |||||
出版タイプResource | http://purl.org/coar/version/c_ab4af688f83e57aa | |||||
DOI | ||||||
関連タイプ | isVersionOf | |||||
識別子タイプ | DOI | |||||
関連識別子 | https://doi.org/10.1021/jacs.7b01965 | |||||
ISSN | ||||||
収録物識別子タイプ | PISSN | |||||
収録物識別子 | 0002-7863 | |||||
書誌情報 |
en : Journal of the American Chemical Society 巻 139, 号 15, p. 5596-5606, 発行日 2017-04-19 |
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著者版フラグ | ||||||
値 | author | |||||
URI | ||||||
識別子 | http://doi.org/10.1021/jacs.7b01965 | |||||
識別子タイプ | DOI | |||||
URI | ||||||
識別子 | http://hdl.handle.net/2237/26770 | |||||
識別子タイプ | HDL |