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Catalytic Ammonia Oxidation to Dinitrogen by a Nickel Complex

Authors: David N. Stephens; Robert K. Szilagyi; Paige N. Roehling; Navamoney Arulsamy; Michael T. Mock;

Catalytic Ammonia Oxidation to Dinitrogen by a Nickel Complex

Abstract

AbstractWe report a nickel complex for catalytic oxidation of ammonia to dinitrogen under ambient conditions. Using the aryloxyl radical 2,4,6‐tri‐tert‐butylphenoxyl (tBu3ArO⋅) as a H atom acceptor to cleave the N−H bond of a coordinated NH3 ligand up to 56 equiv of N2 per Ni center can be generated. Employing the N‐oxyl radical 2,2,6,6‐(tetramethylpiperidin‐1‐yl)oxyl (TEMPO⋅) as the H‐atom acceptor, up to 15 equiv of N2 per Ni center are formed. A bridging Ni‐hydrazine product identified by isotopic nitrogen (15N) studies and supported by computational models indicates the N−N bond forming step occurs by bimetallic homocoupling of two paramagnetic [Ni]−NH2 fragments. Ni‐mediated hydrazine disproportionation to N2 and NH3 completes the catalytic cycle.

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citations
This is an alternative to the "Influence" indicator, which also reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically).
BIP!Citations provided by BIP!
popularity
This indicator reflects the "current" impact/attention (the "hype") of an article in the research community at large, based on the underlying citation network.
BIP!Popularity provided by BIP!
influence
This indicator reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically).
BIP!Influence provided by BIP!
impulse
This indicator reflects the initial momentum of an article directly after its publication, based on the underlying citation network.
BIP!Impulse provided by BIP!
views
OpenAIRE UsageCountsViews provided by UsageCounts
25
Top 10%
Average
Top 10%
4
Green