CO2 Methanation on Cu-Cluster Decorated Zirconia Supports with Different Morphology: A Combined Experimental In Situ GIXANES/GISAXS, Ex Situ XPS and Theoretical DFT Study

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F61388955%3A_____%2F21%3A00543566" target="_blank" >RIV/61388955:_____/21:00543566 - isvavai.cz</a>

Výsledek na webu

<a href="http://hdl.handle.net/11104/0320753" target="_blank" >http://hdl.handle.net/11104/0320753</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1021/acscatal.0c05029" target="_blank" >10.1021/acscatal.0c05029</a>

Jazyk výsledku

angličtina

Název v původním jazyce

CO2 Methanation on Cu-Cluster Decorated Zirconia Supports with Different Morphology: A Combined Experimental In Situ GIXANES/GISAXS, Ex Situ XPS and Theoretical DFT Study

Popis výsledku v původním jazyce

Subnanometer copper tetramer-zirconia catalysts turn out to be highly efficient for CO2 hydrogenation and its conversion to methane. The cluster size and substrate morphology are controlled to optimize the catalytic performance. The two types of zirconia supports investigated are prepared by atomic layer deposition (μ3 nm thick film) and supersonic cluster beam deposition (nanostructured film, μ100 nm thick). The substrate plays a crucial role in determining the activity of the catalyst as well as its cyclability over repeated thermal ramps. A temperature-programmed reaction combined with in situ X-ray characterization reveals the correlation between the evolution in the oxidation state and catalytic activity. Ex situ photoelectron spectroscopy indicates Cu clusters with stronger interactions with the nanostructured film, which can be the cause for the higher activity of this catalyst. Density functional theory calculations based on the Cu4O2 cluster supported on a ZrOx subunit reveal low activation barriers and provide mechanism for CO2 hydrogenation and its conversion to methane. Altogether, the results show a new way to tune the catalytic activity of CO2 hydrogenation catalysts through controlling the morphology of the support at the nanoscale.

Název v anglickém jazyce

CO2 Methanation on Cu-Cluster Decorated Zirconia Supports with Different Morphology: A Combined Experimental In Situ GIXANES/GISAXS, Ex Situ XPS and Theoretical DFT Study

Popis výsledku anglicky

Subnanometer copper tetramer-zirconia catalysts turn out to be highly efficient for CO2 hydrogenation and its conversion to methane. The cluster size and substrate morphology are controlled to optimize the catalytic performance. The two types of zirconia supports investigated are prepared by atomic layer deposition (μ3 nm thick film) and supersonic cluster beam deposition (nanostructured film, μ100 nm thick). The substrate plays a crucial role in determining the activity of the catalyst as well as its cyclability over repeated thermal ramps. A temperature-programmed reaction combined with in situ X-ray characterization reveals the correlation between the evolution in the oxidation state and catalytic activity. Ex situ photoelectron spectroscopy indicates Cu clusters with stronger interactions with the nanostructured film, which can be the cause for the higher activity of this catalyst. Density functional theory calculations based on the Cu4O2 cluster supported on a ZrOx subunit reveal low activation barriers and provide mechanism for CO2 hydrogenation and its conversion to methane. Altogether, the results show a new way to tune the catalytic activity of CO2 hydrogenation catalysts through controlling the morphology of the support at the nanoscale.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10403 - Physical chemistry

Projekt

—

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

ACS Catalysis

ISSN

2155-5435

e-ISSN

2155-5435

Svazek periodika

11

Číslo periodika v rámci svazku

10

Stát vydavatele periodika

US - Spojené státy americké

Počet stran výsledku

15

Strana od-do

6210-6224

Kód UT WoS článku

000656056200032

EID výsledku v databázi Scopus

2-s2.0-85106358211