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

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F61388955%3A_____%2F19%3A00505953" target="_blank" >RIV/61388955:_____/19:00505953 - isvavai.cz</a>

Nalezeny alternativní kódy

RIV/00216275:25310/19:39915344

Výsledek na webu

<a href="http://hdl.handle.net/11104/0297274" target="_blank" >http://hdl.handle.net/11104/0297274</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1038/s42004-019-0173-9" target="_blank" >10.1038/s42004-019-0173-9</a>

Jazyk výsledku

angličtina

Název v původním jazyce

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

Popis výsledku v původním jazyce

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 α-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 α-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.nn

Název v anglickém jazyce

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

Popis výsledku anglicky

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 α-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 α-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.nn

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10403 - Physical chemistry

Projekt

<a href="/cs/project/GA17-00742S" target="_blank" >GA17-00742S: Binukleární struktury iontů v zeolitech</a><br>

Návaznosti

I - Institucionalni podpora na dlouhodoby koncepcni rozvoj vyzkumne organizace

Rok uplatnění

2019

Kód důvěrnosti údajů

S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů

Název periodika

Communications Chemistry

ISSN

2399-3669

e-ISSN

—

Svazek periodika

2

Číslo periodika v rámci svazku

JAN 2019

Stát vydavatele periodika

GB - Spojené království Velké Británie a Severního Irska

Počet stran výsledku

9

Strana od-do

71

Kód UT WoS článku

000472619600001

EID výsledku v databázi Scopus

2-s2.0-85071158227