CO Cleavage and CO₂ Functionalization under Mild Conditions by a Multimetallic CsU₂ Nitride Complex

Area of Science:

• Inorganic Chemistry
• Organometallic Chemistry
• Catalysis

Background:

• Efficient chemical synthesis using abundant feedstocks like carbon dioxide (CO2) and carbon monoxide (CO) is crucial.
• While uranium nitride materials show catalytic activity in the Haber-Bosch process, the reactivity of molecular nitride compounds is underexplored.

Purpose of the Study:

• To investigate the catalytic potential of a specific multimetallic nitride complex for chemical transformations.
• To explore the reactivity of molecular nitride compounds in N-C bond formation and C≡O bond cleavage.

Main Methods:

• Synthesis and characterization of the multimetallic nitride complex [Cs{[U(OSi(OtBu)3)3]2(μ-N)}] (1).
• Evaluation of the complex's reactivity with carbon dioxide (CO2) and carbon monoxide (CO) under mild conditions.

Main Results:

• The CsUIV-N-UIV nitride complex (1) demonstrated strong nucleophile behavior, promoting N-C bond formation.
• Complex 1 reacted with excess CO2 to yield a dicarbamate product.
• The nitride complex effectively cleaved the C≡O bond of carbon monoxide under mild conditions.

Conclusions:

• Molecular nitride complexes, exemplified by the CsUIV-N-UIV nitride, offer promising catalytic pathways for utilizing CO2 and CO.
• This research opens new avenues for developing efficient chemical processes using inexpensive and accessible carbon sources.