Oxygen Splitting and Methane Oxidation over Fe-Mordenite: Insight by the Operando 2D COS UV-Vis-NIR-IR Approach

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F61388955%3A_____%2F24%3A00583973" target="_blank" >RIV/61388955:_____/24:00583973 - isvavai.cz</a>

Výsledek na webu

<a href="https://hdl.handle.net/11104/0351965" target="_blank" >https://hdl.handle.net/11104/0351965</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1021/acs.jpcc.3c08225" target="_blank" >10.1021/acs.jpcc.3c08225</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Oxygen Splitting and Methane Oxidation over Fe-Mordenite: Insight by the Operando 2D COS UV-Vis-NIR-IR Approach

Popis výsledku v původním jazyce

Activation of molecular oxygen and subsequent oxidation of methane over Fe sites in mordenite zeolites with different content of framework Al atoms were studied in the continuous regime at low temperatures. For this purpose, reactivity tests of methane oxidation by molecular oxygen over iron mordenite zeolites were combined with an operando 2D COS UV-vis-NIR-IR study to analyze the reaction pathway. The transmission spectra in the visible-NIR-IR range of investigated iron mordenites revealed the structural changes of Fe(II) after O2 treatment and the formation of the spectral features typical for alpha-O stabilized on iron. Mass spectrometry analysis of gaseous products of the simultaneous interaction of methane and oxygen with iron mordenite revealed the formation of methanol, water, carbon monoxide, and carbon dioxide. Moreover, operando 2D COS UV-vis-NIR-IR also evidenced the presence of formaldehyde, formate, carbon dioxide, and carbon monoxide as products of subsequent methanol oxidation. The differences in the reaction pathway of methane oxidation over Fe-mordenite compared to Fe-ferrierite and Fe-*BEA catalysts reflect unique properties of mordenite topology providing isolated alpha-oxygens in individual mordenite pockets, although formed by splitting of molecular oxygen by two cooperating iron ions and the nature of adsorption sites in the mordenite matrix.

Název v anglickém jazyce

Oxygen Splitting and Methane Oxidation over Fe-Mordenite: Insight by the Operando 2D COS UV-Vis-NIR-IR Approach

Popis výsledku anglicky

Activation of molecular oxygen and subsequent oxidation of methane over Fe sites in mordenite zeolites with different content of framework Al atoms were studied in the continuous regime at low temperatures. For this purpose, reactivity tests of methane oxidation by molecular oxygen over iron mordenite zeolites were combined with an operando 2D COS UV-vis-NIR-IR study to analyze the reaction pathway. The transmission spectra in the visible-NIR-IR range of investigated iron mordenites revealed the structural changes of Fe(II) after O2 treatment and the formation of the spectral features typical for alpha-O stabilized on iron. Mass spectrometry analysis of gaseous products of the simultaneous interaction of methane and oxygen with iron mordenite revealed the formation of methanol, water, carbon monoxide, and carbon dioxide. Moreover, operando 2D COS UV-vis-NIR-IR also evidenced the presence of formaldehyde, formate, carbon dioxide, and carbon monoxide as products of subsequent methanol oxidation. The differences in the reaction pathway of methane oxidation over Fe-mordenite compared to Fe-ferrierite and Fe-*BEA catalysts reflect unique properties of mordenite topology providing isolated alpha-oxygens in individual mordenite pockets, although formed by splitting of molecular oxygen by two cooperating iron ions and the nature of adsorption sites in the mordenite matrix.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10403 - Physical chemistry

Projekt

<a href="/cs/project/GA22-06737S" target="_blank" >GA22-06737S: Aktivace molekulárního dusíku</a><br>

Návaznosti

I - Institucionalni podpora na dlouhodoby koncepcni rozvoj vyzkumne organizace

Rok uplatnění

2024

Kód důvěrnosti údajů

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

Název periodika

Journal of Physical Chemistry C

ISSN

1932-7447

e-ISSN

1932-7455

Svazek periodika

128

Číslo periodika v rámci svazku

9

Stát vydavatele periodika

US - Spojené státy americké

Počet stran výsledku

11

Strana od-do

3759-3769

Kód UT WoS článku

001173716500001

EID výsledku v databázi Scopus

2-s2.0-85186069862