A Bioinspired Iron-Molybdenum µ-Nitrido Complex and Its Reactivity toward Ammonia Formation.
Angew Chem Int Ed Engl
; 61(30): e202203121, 2022 07 25.
Article
em En
| MEDLINE
| ID: mdl-35604770
ABSTRACT
Multimetallic nitride species, especially those containing biologically related iron or molybdenum, are fundamentally important to understand the nitrogen reduction process catalysed by FeMo-nitrogenase. However, until now, there remains no report about the construction of structurally well-defined FeMo heteronuclear nitrido complex and its reactivity toward ammonia formation. Herein, a novel thiolate-bridged FeII MoVI complex featuring a bent Fe-N≡Mo fragment is synthesized and structurally characterized, which can be easily protonated to form a µ-imido complex. Subsequently, through the proton-coupled electron transfer (PCET) process, this imido species can smoothly convert into the µ-amido complex, which can further undergo reductive protonation to afford the FeMo complex containing an ammine ligand. Overall, we present the first well-defined {Fe(µ-S)2 Mo} platform that can give a panoramic picture for the late stage (N3- âNH2- âNH2- âNH3 ) of biological nitrogen reduction by the heterometallic cooperativity.
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Texto completo:
1
Coleções:
01-internacional
Base de dados:
MEDLINE
Assunto principal:
Amônia
/
Molibdênio
Idioma:
En
Ano de publicação:
2022
Tipo de documento:
Article