Formation of C1 oxygenates by Activation of Methane on B, N Co-doped Graphene Surface Decorated by Oxygen Pre-covered Ir13 Cluster: A First Principles Study

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F49777513%3A23520%2F25%3A43975497" target="_blank" >RIV/49777513:23520/25:43975497 - isvavai.cz</a>

Výsledek na webu

<a href="https://doi.org/10.1002/open.202400287" target="_blank" >https://doi.org/10.1002/open.202400287</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1002/open.202400287" target="_blank" >10.1002/open.202400287</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Formation of C1 oxygenates by Activation of Methane on B, N Co-doped Graphene Surface Decorated by Oxygen Pre-covered Ir13 Cluster: A First Principles Study

Popis výsledku v původním jazyce

The environmentally friendly conversion of methane to value-added chemicals is studied by ab-initio calculations. We focus on the adsorption and dehydrogenation of methane were investigated on Ir13 cluster supported by boron nitrogen co-doped graphene (BNG). We show that the BNG-Ir13 cluster with low oxygen coverage exhibits more negative adsorption energy of methane (−0.44 eV) and lower activation energy barrier for its dissociation (1.24 eV for the second dehydrogenation step) compared to the cluster with high oxygen coverage. Next, assuming abundant CH3 and CH2 species due to a proper temperature control preventing further dehydrogenation, we study competitive C–O coupling reactions leading to the formation of value-added chemicals. The activation energy barriers for the formation of methanol and formaldehyde are on BNG-Ir13 are once again lower at a lower oxygen coverage. Furthermore, we study hydrogen recombination and confirm that H2 molecules can be formed on these surfaces. Based on these findings, the low-oxygen-coverage BNG-Ir13 cluster emerges as a promising catalyst for the selective conversion of methane to methanol and formaldehyde, as well as for hydrogen production.

Název v anglickém jazyce

Formation of C1 oxygenates by Activation of Methane on B, N Co-doped Graphene Surface Decorated by Oxygen Pre-covered Ir13 Cluster: A First Principles Study

Popis výsledku anglicky

The environmentally friendly conversion of methane to value-added chemicals is studied by ab-initio calculations. We focus on the adsorption and dehydrogenation of methane were investigated on Ir13 cluster supported by boron nitrogen co-doped graphene (BNG). We show that the BNG-Ir13 cluster with low oxygen coverage exhibits more negative adsorption energy of methane (−0.44 eV) and lower activation energy barrier for its dissociation (1.24 eV for the second dehydrogenation step) compared to the cluster with high oxygen coverage. Next, assuming abundant CH3 and CH2 species due to a proper temperature control preventing further dehydrogenation, we study competitive C–O coupling reactions leading to the formation of value-added chemicals. The activation energy barriers for the formation of methanol and formaldehyde are on BNG-Ir13 are once again lower at a lower oxygen coverage. Furthermore, we study hydrogen recombination and confirm that H2 molecules can be formed on these surfaces. Based on these findings, the low-oxygen-coverage BNG-Ir13 cluster emerges as a promising catalyst for the selective conversion of methane to methanol and formaldehyde, as well as for hydrogen production.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10403 - Physical chemistry

Projekt

<a href="/cs/project/EH22_008%2F0004572" target="_blank" >EH22_008/0004572: Kvantové materiály pro aplikace v udržitelných technologiích</a><br>

Návaznosti

P - Projekt vyzkumu a vyvoje financovany z verejnych zdroju (s odkazem do CEP)<br>I - Institucionalni podpora na dlouhodoby koncepcni rozvoj vyzkumne organizace

Rok uplatnění

2025

Kód důvěrnosti údajů

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

Název periodika

ChemistryOpen

ISSN

2191-1363

e-ISSN

2191-1363

Svazek periodika

14

Číslo periodika v rámci svazku

5

Stát vydavatele periodika

DE - Spolková republika Německo

Počet stran výsledku

10

Strana od-do

nestránkováno

Kód UT WoS článku

001420903900001

EID výsledku v databázi Scopus

2-s2.0-85217659744