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単核非ヘム鉄複合体による二酸化物の活性化: 連続的なペロクソ,オクソ,およびヒドロクソ中間体

Jesse B Gordon¹, Avery C Vilbert², Ida M DiMucci²

¹Department of Chemistry , The Johns Hopkins University , 3400 North Charles Street , Baltimore , Maryland 21218 , United States.

Journal of the American Chemical Society

|October 25, 2019

まとめ

この研究では,Fe^III - O-O-Fe^IIIとFe^IV^{O) の中間体を形成する単核非ヘム鉄^II複合体によるダイオキシゲン活性化が報告されています. この研究は,硫黄リガンドを鉄酸素化学で使用する可能性を実証している.}

科学分野:

バイオ有機化学
有機金属化学
協調化学

背景:

非ヘム鉄複合体による二酸化炭素の活性化は,生物学的プロセスと触媒に不可欠である.
効率的な触媒の設計には鉄酸素中間物質の仕組みを理解することが重要です
単核非ヘム鉄システムは,複雑な反応性を研究するための簡素化されたモデルを提供します.

研究の目的:

硫黄ドナーリガンドによる単核非ヘム鉄 (II) 複合体によるダイオキシゲンの活性化を調査する.
鉄酸化物と高価鉄酸化物を含む鉄酸化物の中間物質の特徴を明らかにする.
これらの中間物質の反応性とその触媒への影響を探求する.

主な方法:

UV-vis,Mössbauer,共振ラマン (RR),X線吸収 (XAS) スペクトルスコピーを用いて鉄複合体の合成と特徴付け.
低温でダイオキシゲンで反応し,反応性中間物質を生成し,分離する.
鉄-酸素種の構造と変換を明らかにするための光譜と反応性研究.

主要な成果:

O_{2と反応したチオラート結合 (ペロキソ) 鉄複合体 (Fe^III₂(O₂) の形成.}
ペロキソ介質のO−O結合割れによるFe^IV(O) 種の生成.
Fe^III(OH) の形成をH原子ドナーからFe^IV(O) 種から観察した.
安定したFe/O₂中間物質と硫黄リガンドの立即酸化を証明する.

結論:

この研究は,単核非ヘム鉄 (II) 複合体によるダイオキシゲン活性化の希少な例を示している.
この研究は,同じ反応でFe^III-O-Fe^IIIとFe^IV(O) の両種を成功裏に生成し,特徴づけました.
この発見は,反応性鉄と酸素の中間物質の安定化における強い硫黄のリガンドの役割を強調している.

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