2019年3月1日
Site-Selective Supramolecular Complexation Activates Catalytic Ethane Oxidation by a Nitrido-Bridged Iron Porphyrinoid Dimer
Chemistry - A European Journal
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- 巻
- 25
- 号
- 13
- 開始ページ
- 3369
- 終了ページ
- 3375
- 記述言語
- 英語
- 掲載種別
- 研究論文(学術雑誌)
- DOI
- 10.1002/chem.201805580
- 出版者・発行元
- WILEY-V C H VERLAG GMBH
© 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim Development of supramolecular methods to further activate a highly reactive intermediate is a fascinating strategy to create novel potent catalysts for activation of inert chemicals. Herein, a supramolecular approach to enhance the oxidizing ability of a high-valent oxo species of a nitrido-bridged iron porphyrinoid dimer that is a known potent molecular catalyst for light alkane oxidation is reported. For this purpose, a nitrido-bridged dinuclear iron complex of porphyrin-phthalocyanine heterodimer 3 5+ , which is connected through a fourfold rotaxane, was prepared. Heterodimer 3 5+ catalyzed ethane oxidation in the presence of H 2 O 2 at a relatively low temperature. The site-selective complexation of 3 5+ with an additional anionic porphyrin (TPPS 4− ) through π–π stacking and electrostatic interactions afforded a stable 1:1 complex. It was demonstrated that the supramolecular post-synthetic modification of 3 5+ enhances its catalytic activity efficiently. Moreover, supramolecular conjugates achieved higher catalytic ethane oxidation activity than nitrido-bridged iron phthalocyanine dimer, which is the most potent iron-oxo-based molecular catalyst for light-alkane oxidation reported so far. Electrochemical measurements proved that the electronic perturbation from TPPS 4− to 3 5+ enhanced the catalytic activity.
- リンク情報
- ID情報
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- DOI : 10.1002/chem.201805580
- ISSN : 1521-3765
- ISSN : 0947-6539
- eISSN : 1521-3765
- ORCIDのPut Code : 91509770
- PubMed ID : 30548706
- SCOPUS ID : 85061280209