Fe-Hydrazido休息状態経由でN₂をN(SiMe₃) ₃に変換する

Adam D Piascik¹, Ruohao Li¹, Harry J Wilkinson¹

¹Department of Chemistry , Imperial College London , Exhibition Road , South Kensington, London SW7 2AZ , United Kingdom.

Journal of the American Chemical Society

|August 18, 2018

まとめ

鉄触媒は窒素ガス (N₂) をシリ化アミンに効率的に変換し,記録的な収量を達成します. 機理学的な研究は,中間シリレーション,還元,不釣り合いを伴う経路を明らかにし,N-N結合割れが続く.

科学分野:

均質な触媒
有機金属化学
窒素固定

背景:

N₂を有価な製品に触媒的に変換することは極めて重要です.
N₂活性化のための3D移行金属触媒のメカニズムに関する理解は限られている.

研究の目的:

N₂変換のための鉄複合体の触媒機構を調査する.
N_{2からN_{3_{の生産で高い収穫量を達成する.}}}

主な方法:

使用された鉄複合体Fe (PP) ₂ (N₂) と PP = R₂PCH₂CH₂PR₂ (R = Me, Et) を含む.
カリウムグラフィート (KC₈) とトリメチルシリル塩化物 (Me₃SiCl) を反応剤として使用した.
密度関数理論 (DFT) の計算を組み合わせた実験研究.

主要な成果:

N_{2からN (SiMe₃) ₃の生産で,鉄ベースの触媒で報告された最も高い収量を達成しました.}
Fe^I(NN-SiMe₃) 中間物質を形成するために,電離性N_βシリレーションと1e^-還元を含むメカニズムを提案した.
識別されたFe^II[N-N(SiMe₃) ₂種は,触媒的な休息状態であり,N-N結合分裂が続く.

結論:

Fe (PP) ₂ (N₂) 複合体は,N₂変換のための非常に効果的な触媒である.
提案されたメカニズムは,3D金属触媒によるN₂固定に鍵となるメカニズム的な洞察を提供します.
実験データと計算データは,解明された触媒サイクルを支持する.

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Fe-Hydrazido休息状態経由でN2をN(SiMe3) 3に変換する