Splitting dioxygen over distant binuclear transition metal cationic sites in zeolites. Effect of the transition metal cation

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F61388955%3A_____%2F21%3A00539847" target="_blank" >RIV/61388955:_____/21:00539847 - isvavai.cz</a>

Nalezeny alternativní kódy

RIV/86652036:_____/21:00542511

Výsledek na webu

<a href="http://hdl.handle.net/11104/0317548" target="_blank" >http://hdl.handle.net/11104/0317548</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1002/qua.26611" target="_blank" >10.1002/qua.26611</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Splitting dioxygen over distant binuclear transition metal cationic sites in zeolites. Effect of the transition metal cation

Popis výsledku v původním jazyce

Splitting dioxygen to yield highly active oxygen species attracts enormous attention due to its potential in direct oxidation reactions, mainly in transformation of methane into valuable products. Distant binuclear cationic Fe(II) centers in Fe-ferrierite have recently been shown to be active in splitting dioxygen at room temperature to form very active oxygen species able to oxidize methane to methanol at room temperature as well. Computational models of the distant binuclear transition metal cationic sites (Co(II), Mn(II), and Fe(II)) stabilized in the ferrierite matrix were investigated by periodic density-functional theory calculations including molecular dynamics simulations. The results reveal that the M(II) cations capable of the M(II)> M(IV) redox cycle with the M horizontal ellipsis M distance of ca 7.4 angstrom stabilized in two adjacent beta sites of ferrierite can split dioxygen. Our study opens the possibility of developing tunable zeolite-based systems for the activation of dioxygen employed for direct oxidations.

Název v anglickém jazyce

Splitting dioxygen over distant binuclear transition metal cationic sites in zeolites. Effect of the transition metal cation

Popis výsledku anglicky

Splitting dioxygen to yield highly active oxygen species attracts enormous attention due to its potential in direct oxidation reactions, mainly in transformation of methane into valuable products. Distant binuclear cationic Fe(II) centers in Fe-ferrierite have recently been shown to be active in splitting dioxygen at room temperature to form very active oxygen species able to oxidize methane to methanol at room temperature as well. Computational models of the distant binuclear transition metal cationic sites (Co(II), Mn(II), and Fe(II)) stabilized in the ferrierite matrix were investigated by periodic density-functional theory calculations including molecular dynamics simulations. The results reveal that the M(II) cations capable of the M(II)> M(IV) redox cycle with the M horizontal ellipsis M distance of ca 7.4 angstrom stabilized in two adjacent beta sites of ferrierite can split dioxygen. Our study opens the possibility of developing tunable zeolite-based systems for the activation of dioxygen employed for direct oxidations.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10403 - Physical chemistry

Projekt

Výsledek vznikl pri realizaci vícero projektů. Více informací v záložce Projekty.

Návaznosti

I - Institucionalni podpora na dlouhodoby koncepcni rozvoj vyzkumne organizace

Rok uplatnění

2021

Kód důvěrnosti údajů

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

Název periodika

International Journal of Quantum Chemistry

ISSN

0020-7608

e-ISSN

1097-461X

Svazek periodika

121

Číslo periodika v rámci svazku

10

Stát vydavatele periodika

US - Spojené státy americké

Počet stran výsledku

7

Strana od-do

e26611

Kód UT WoS článku

000614366800001

EID výsledku v databázi Scopus

2-s2.0-85100472144