Nitrogen fixation catalyzed by ferrocene-substituted dinitrogen-bridged dimolybdenum-dinitrogen complexes: Unique behavior of ferrocene moiety as redox active site

Shogo Kuriyama, Kazuya Arashiba, Kazunari Nakajima, Hiromasa Tanaka, Kazunari Yoshizawa, Yoshiaki Nishibayashi

研究成果: ジャーナルへの寄稿記事

54 引用 (Scopus)

抄録

A series of dinitrogen-bridged dimolybdenum-dinitrogen complexes bearing metallocene-substituted PNP-pincer ligands is synthesized by the reduction of the corresponding monomeric molybdenum-trichloride complexes under 1 atm of molecular dinitrogen. Introduction of ferrocene as a redox-active moiety to the pyridine ring of the PNP-pincer ligand increases the catalytic activity for the formation of ammonia from molecular dinitrogen, up to 45 equiv. of ammonia being formed based on the catalyst (22 equiv. of ammonia based on each molybdenum atom of the catalyst). The time profile for the catalytic reaction reveals that the presence of the ferrocene unit in the catalyst increases the rate of ammonia formation. Electrochemical measurement and theoretical studies indicate that an interaction between the Fe atom of the ferrocene moiety and the Mo atom in the catalyst may play an important role to achieve a high catalytic activity.

元の言語英語
ページ(範囲)3940-3951
ページ数12
ジャーナルChemical Science
6
発行部数7
DOI
出版物ステータス出版済み - 7 1 2015

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Nitrogen fixation
Ammonia
Catalysts
Molybdenum
Atoms
Catalyst activity
Bearings (structural)
Ligands
Oxidation-Reduction
ferrocene

All Science Journal Classification (ASJC) codes

  • Chemistry(all)

これを引用

Nitrogen fixation catalyzed by ferrocene-substituted dinitrogen-bridged dimolybdenum-dinitrogen complexes : Unique behavior of ferrocene moiety as redox active site. / Kuriyama, Shogo; Arashiba, Kazuya; Nakajima, Kazunari; Tanaka, Hiromasa; Yoshizawa, Kazunari; Nishibayashi, Yoshiaki.

:: Chemical Science, 巻 6, 番号 7, 01.07.2015, p. 3940-3951.

研究成果: ジャーナルへの寄稿記事

Kuriyama, Shogo ; Arashiba, Kazuya ; Nakajima, Kazunari ; Tanaka, Hiromasa ; Yoshizawa, Kazunari ; Nishibayashi, Yoshiaki. / Nitrogen fixation catalyzed by ferrocene-substituted dinitrogen-bridged dimolybdenum-dinitrogen complexes : Unique behavior of ferrocene moiety as redox active site. :: Chemical Science. 2015 ; 巻 6, 番号 7. pp. 3940-3951.
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abstract = "A series of dinitrogen-bridged dimolybdenum-dinitrogen complexes bearing metallocene-substituted PNP-pincer ligands is synthesized by the reduction of the corresponding monomeric molybdenum-trichloride complexes under 1 atm of molecular dinitrogen. Introduction of ferrocene as a redox-active moiety to the pyridine ring of the PNP-pincer ligand increases the catalytic activity for the formation of ammonia from molecular dinitrogen, up to 45 equiv. of ammonia being formed based on the catalyst (22 equiv. of ammonia based on each molybdenum atom of the catalyst). The time profile for the catalytic reaction reveals that the presence of the ferrocene unit in the catalyst increases the rate of ammonia formation. Electrochemical measurement and theoretical studies indicate that an interaction between the Fe atom of the ferrocene moiety and the Mo atom in the catalyst may play an important role to achieve a high catalytic activity.",
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AU - Kuriyama, Shogo

AU - Arashiba, Kazuya

AU - Nakajima, Kazunari

AU - Tanaka, Hiromasa

AU - Yoshizawa, Kazunari

AU - Nishibayashi, Yoshiaki

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N2 - A series of dinitrogen-bridged dimolybdenum-dinitrogen complexes bearing metallocene-substituted PNP-pincer ligands is synthesized by the reduction of the corresponding monomeric molybdenum-trichloride complexes under 1 atm of molecular dinitrogen. Introduction of ferrocene as a redox-active moiety to the pyridine ring of the PNP-pincer ligand increases the catalytic activity for the formation of ammonia from molecular dinitrogen, up to 45 equiv. of ammonia being formed based on the catalyst (22 equiv. of ammonia based on each molybdenum atom of the catalyst). The time profile for the catalytic reaction reveals that the presence of the ferrocene unit in the catalyst increases the rate of ammonia formation. Electrochemical measurement and theoretical studies indicate that an interaction between the Fe atom of the ferrocene moiety and the Mo atom in the catalyst may play an important role to achieve a high catalytic activity.

AB - A series of dinitrogen-bridged dimolybdenum-dinitrogen complexes bearing metallocene-substituted PNP-pincer ligands is synthesized by the reduction of the corresponding monomeric molybdenum-trichloride complexes under 1 atm of molecular dinitrogen. Introduction of ferrocene as a redox-active moiety to the pyridine ring of the PNP-pincer ligand increases the catalytic activity for the formation of ammonia from molecular dinitrogen, up to 45 equiv. of ammonia being formed based on the catalyst (22 equiv. of ammonia based on each molybdenum atom of the catalyst). The time profile for the catalytic reaction reveals that the presence of the ferrocene unit in the catalyst increases the rate of ammonia formation. Electrochemical measurement and theoretical studies indicate that an interaction between the Fe atom of the ferrocene moiety and the Mo atom in the catalyst may play an important role to achieve a high catalytic activity.

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