In:
Angewandte Chemie, Wiley, Vol. 134, No. 30 ( 2022-07-25)
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 Fe II Mo VI 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 (N 3− →NH 2− →NH 2 − →NH 3 ) of biological nitrogen reduction by the heterometallic cooperativity.
Type of Medium:
Online Resource
ISSN:
0044-8249
,
1521-3757
DOI:
10.1002/ange.v134.30
DOI:
10.1002/ange.202203121
Language:
English
Publisher:
Wiley
Publication Date:
2022
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