In-situ DRIFTS and NAP-XPS exploration of the complexity of CO2 hydrogenation over size controlled Pt nanoparticles supported on mesoporous NiO

4.8 nm Pt nanoparticles were anchored onto the surface of mesoporous nickel-oxide supports (NiO). Pt/NiO samples were compared to pristine NiO and Pt/SBA-15 silica catalysts in CO2 hydrogenation to form carbon-monoxide, methane and ethane at 473-673 K. 1 % Pt/NiO were ~20 times and ~1.5 times more a...

Teljes leírás

Elmentve itt :
Bibliográfiai részletek
Szerzők: Sápi András
Halasi Gyula
Kiss János
Dobó Dorina Gabriella
Juhász Koppány Levente
Kolcsár Vanessza J.
Ferencz Zsuzsa
Vári Gábor
Matolin Vladimír
Erdőhelyi András
Kukovecz Ákos
Kónya Zoltán
Dokumentumtípus: Cikk
Megjelent: American Chemical Society 2018
Sorozat:JOURNAL OF PHYSICAL CHEMISTRY C 122 No. 10
Tárgyszavak:
doi:10.1021/acs.jpcc.8b00061

mtmt:3339431
Online Access:http://publicatio.bibl.u-szeged.hu/13120
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520 3 |a 4.8 nm Pt nanoparticles were anchored onto the surface of mesoporous nickel-oxide supports (NiO). Pt/NiO samples were compared to pristine NiO and Pt/SBA-15 silica catalysts in CO2 hydrogenation to form carbon-monoxide, methane and ethane at 473-673 K. 1 % Pt/NiO were ~20 times and ~1.5 times more active at 493 K compared to Pt/SBA-15 and NiO catalysts, respectively. However, the Pt-free NiO support has an activity of 120% compared to Pt/NiO catalysts at 673 K. In the case of 1% Pt/SBA-15 catalyst, selectivity towards methane was 13 %, while it was 90% and 98% for NiO and 1% Pt/NiO at 673 K, respectively. Exploration of the results of the reactions was performed by Near Ambient Pressure X-ray Photoelectron Spectroscopy (NAP-XPS) as well as in-situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS). In the case of pure NiO, we found that the surface of the support was mainly covered by elemental Ni under reaction condition, where the Ni/NiOx system is responsible for the high activity of Pt-free catalyst. In the case of Pt/NiO, Pt improves the reduction of NiOx towards metallic Ni. In the case of the 1 % Pt/NiO catalysts, the presence of limited amount of Pt resulted in an optimal quantity of oxidized Pt fraction at 673 K showing the presence of a Pt/PtOx/Ni/NiOx mixed phase where the different interfaces may be responsible for the high activity and selectivity towards methane. In the case of pure NiO under reaction condition, small amounts of formaldehyde as well as hydrogen perturbed CO [HnCO (n=1,2)] were detected. However, in the case of 1 % Pt/NiO catalysts, besides the absence of formaldehyde a significant amount of HnCO (n=2-3) was present on the surface responsible for the high activity and methane selectivity. 
650 4 |a Kémiai tudományok 
700 0 1 |a Halasi Gyula  |e aut 
700 0 1 |a Kiss János  |e aut 
700 0 1 |a Dobó Dorina Gabriella  |e aut 
700 0 1 |a Juhász Koppány Levente  |e aut 
700 0 1 |a Kolcsár Vanessza J.  |e aut 
700 0 1 |a Ferencz Zsuzsa  |e aut 
700 0 1 |a Vári Gábor  |e aut 
700 0 1 |a Matolin Vladimír  |e aut 
700 0 1 |a Erdőhelyi András  |e aut 
700 0 1 |a Kukovecz Ákos  |e aut 
700 0 1 |a Kónya Zoltán  |e aut 
856 4 0 |u http://publicatio.bibl.u-szeged.hu/13120/1/JPC_C12220185553_u.pdf  |z Dokumentum-elérés