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Fast Hydrocarbon Oxidation by a High-Valent Nickel-Fluoride Complex
Prasenjit Mondal1, Marta Lovisari1, Brendan Twamley1
1School of Chemistry, Trinity College Dublin, The University of Dublin, College Green, Dublin, 2, Ireland.
High-valent nickel-fluoride complexes demonstrate potent oxidizing capabilities. These novel compounds facilitate efficient hydrocarbon oxidation and fluorination via a hydrogen atom transfer mechanism.
Area of Science:
- Inorganic Chemistry
- Oxidation Chemistry
- Catalysis
Background:
- Development of potent oxidants is crucial for chemical synthesis.
- High-valent metal-fluoride complexes are explored as potential reactive species.
Purpose of the Study:
- To synthesize and characterize a high-valent nickel-fluoride complex.
- To evaluate its efficacy as an oxidant for hydrocarbon transformations.
Main Methods:
- Synthesis of nickel-fluoride complexes [NiII (F)(L)]- (1) and [NiIII (F)(L)] (2).
- Characterization using NMR, UV-vis, EPR, mass spectrometry, and X-ray crystallography.
- Kinetic studies and product analysis for oxidation reactions.
Main Results:
- Complex 2, a high-valent Ni-F complex, was successfully prepared and characterized.
- Complex 2 exhibited high reactivity as an oxidant, particularly in hydrocarbon oxidation.
- A hydrogen atom transfer mechanism was identified, with significant rate enhancements compared to related chloro-complexes.
Conclusions:
- High-valent metal-fluorides represent a promising class of potent oxidants.
- Complex 2 serves as an effective catalyst for hydrocarbon oxidation and fluorination.
- These findings offer a new avenue for designing catalysts in oxidation and fluorination chemistry.
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