1. Dioxygen dissociation over man-made system at room temperature to form the active α-oxygen for methane oxidation
- Author
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Tabor, Edyta, Dedecek, Jiri, Mlekodaj, Kinga, Sobalik, Zdenek, Andrikopoulos, Prokopis C., and Sklenak, Stepan
- Subjects
inorganic chemicals ,Multidisciplinary ,biology ,010405 organic chemistry ,Materials Science ,SciAdv r-articles ,Active site ,chemistry.chemical_element ,010402 general chemistry ,Photochemistry ,01 natural sciences ,Redox ,Oxygen ,Methane ,Dissociation (chemistry) ,0104 chemical sciences ,Catalysis ,chemistry.chemical_compound ,chemistry ,Anaerobic oxidation of methane ,biology.protein ,Methanol ,Research Articles ,Research Article - Abstract
Highly active and stable inorganic material for dissociation of dioxygen and methane oxidation to methanol was developed., Activation of dioxygen attracts enormous attention due to its potential for utilization of methane and applications in other selective oxidation reactions. We report a cleavage of dioxygen at room temperature over distant binuclear Fe(II) species stabilized in an aluminosilicate matrix. A pair of formed distant α-oxygen species [i.e., (Fe(IV)═O)2+] exhibits unique oxidation properties reflected in an outstanding activity in the oxidation of methane to methanol at room temperature. Designing a man-made system that mimicks the enzyme functionality in the dioxygen activation using both a different mechanism and structure of the active site represents a breakthrough in catalysis. Our system has an enormous practical importance as a potential industrial catalyst for methane utilization because (i) the Fe(II)/Fe(IV) cycle is reversible, (ii) the active Fe centers are stable under the reaction conditions, and (iii) methanol can be released to gas phase without the necessity of water or water-organic medium extraction.
- Published
- 2020