Low-temperature selective oxidation of methane over distant binuclear cationic centers in zeolites

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dc.contributor.author Tabor, Edyta cze
dc.contributor.author Lemishka, Mariia cze
dc.contributor.author Sobalik, Zdenek cze
dc.contributor.author Mlekodaj, Kinga cze
dc.contributor.author Andrikopoulos, Prokopis C. cze
dc.contributor.author Dedecek, Jiri cze
dc.contributor.author Sklenak, Stepan cze
dc.date.accessioned 2020-03-19T12:42:58Z
dc.date.available 2020-03-19T12:42:58Z
dc.date.issued 2019 eng
dc.identifier.issn 2399-3669 eng
dc.identifier.uri https://hdl.handle.net/10195/74841
dc.description.abstract Highly active oxygen capable to selectively oxidize methane to methanol at low temperature can be prepared in transition-metal cation exchanged zeolites. Here we show that the alpha-oxygen stabilized by the negative charges of two framework aluminum atoms can be prepared by the dissociation of nitrous oxide over distant binuclear cation structures (M(II) ... M (II), M = cobalt, nickel, and iron) accommodated in two adjacent 6-rings forming cationic sites in the ferrierite zeolite. This alpha-oxygen species is analogous to that known only for iron exchanged zeolites. In contrast to divalent iron cations, only binuclear divalent cobalt cationic structures and not isolated divalent cobalt cations are active. Created methoxy moieties are easily protonated to yield methanol, formaldehyde, and formic acid which are desorbed to the gas phase without the aid of water vapor while previous studies showed that highly stable methoxy groups were formed on isolated iron cations in iron exchanged ZSM-5 zeolites. eng
dc.format p. 71-1-71-9 eng
dc.language.iso eng eng
dc.publisher Nature Publishing Group eng
dc.relation.ispartof Communications Chemistry, volume 2, issue: June eng
dc.rights open access eng
dc.rights.uri https://creativecommons.org/licenses/by/4.0/
dc.subject initio molecular-dynamics eng
dc.subject total-energy calculations eng
dc.subject o-t vibrations eng
dc.subject n2o decomposition eng
dc.subject computer experiments eng
dc.subject classical fluids eng
dc.subject periodic dft eng
dc.subject alpha-sites eng
dc.subject fe-bea eng
dc.subject benzene eng
dc.subject molekulární dynamika cze
dc.subject DFT cze
dc.subject zeolit cze
dc.subject selektivní oxidace cze
dc.subject přechodné kovy cze
dc.title Low-temperature selective oxidation of methane over distant binuclear cationic centers in zeolites eng
dc.title.alternative Nízkoteplotní selektivní oxidace metanu na vzdálených binukleárních kationtových centrech zeolitů cze
dc.type article eng
dc.description.abstract-translated Vysoce aktivní kyslík dostupný pro selektivní oxidaci metanu na metanol při nízkých teplotách může být připraven iontovou výměnou v zeolitech. cze
dc.peerreviewed yes eng
dc.publicationstatus published version eng
dc.identifier.doi 10.1038/s42004-019-0173-9 eng
dc.relation.publisherversion https://www.nature.com/articles/s42004-019-0173-9 eng
dc.project.ID SGS_2019_004/Speciální materiály pro chemickou a farmaceutickou technologii a další aplikace eng
dc.identifier.wos 000472619600001 eng
dc.identifier.scopus 2-s2.0-85071158227
dc.identifier.obd 39883846 eng


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