Dioxygen dissociation over man-made system at room temperature to form the active α-oxygen for methane oxidation

0524418 - ÚFCH JH 2021 RIV US eng J - Článek v odborném periodiku
Tabor, Edyta - Dědeček, Jiří - Mlekodaj, Kinga - Sobalík, Zdeněk - Andrikopoulos, Prokopis C. - Sklenák, Štěpán
Dioxygen dissociation over man-made system at room temperature to form the active α-oxygen for methane oxidation.
Science Advances. Roč. 6, č. 20 (2020), č. článku eaa9776. ISSN 2375-2548. E-ISSN 2375-2548
Grant CEP: GA ČR(CZ) GA17-00742S
Grant ostatní: Ga MŠk(CZ) LM2015070
Institucionální podpora: RVO:61388955
Klíčová slova: INITIO MOLECULAR-DYNAMICS * N2O DECOMPOSITION * SELECTIVE OXIDATION
Obor OECD: Physical chemistry
Impakt faktor: 14.143, rok: 2020
Způsob publikování: Open access

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 -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.
Trvalý link: http://hdl.handle.net/11104/0308778