CO2 hydrogenation was carried out over Pt-containing UiO-67 Zr-MOFs at T = 220280 degrees C and ambient pressure, with H-2/CO2 = 0.29 and contact times, tau = 0.0040.01 gcat.min.mL1. The catalysts were characterized by XRD, N-2 adsorption, FESEM, TEM and HRTEM, Pt L-3-edge XANES and EXAFS, dissolution-NMR, CO chemisorption, IR spectroscopy, and TGA. A positive correlation was observed between the degree of Pt reduction and CO2 conversion. Contact time variation experiments showed that CO is a primary product of reaction, while CH4 is a secondary product. Testing of catalyst crystals with 0.15 and 2.0 mu m crystal size, respectively, revealed no influence of diffusion on the reaction rate. Comparison to a conventional Pt/SiO2 catalyst showed very similar activation energy, with E-app = 50 +/- 3 kJ.mol(-1). However, the turnover frequency over Pt/SiO2 was significantly lower, and Pt/SiO2 did not yield methane as a product. The Pt-containing UiO-67 Zr-MOF catalyst showed stable activity during 60 h of testing.

CO2 Hydrogenation over Pt-Containing UiO-67 Zr-MOFs - The Base Case

Manzoli, Maela;Braglia, Luca;Lazzarini, Andrea;Borfecchia, Elisa;Lamberti, Carlo;Bordiga, Silvia;
2017-01-01

Abstract

CO2 hydrogenation was carried out over Pt-containing UiO-67 Zr-MOFs at T = 220280 degrees C and ambient pressure, with H-2/CO2 = 0.29 and contact times, tau = 0.0040.01 gcat.min.mL1. The catalysts were characterized by XRD, N-2 adsorption, FESEM, TEM and HRTEM, Pt L-3-edge XANES and EXAFS, dissolution-NMR, CO chemisorption, IR spectroscopy, and TGA. A positive correlation was observed between the degree of Pt reduction and CO2 conversion. Contact time variation experiments showed that CO is a primary product of reaction, while CH4 is a secondary product. Testing of catalyst crystals with 0.15 and 2.0 mu m crystal size, respectively, revealed no influence of diffusion on the reaction rate. Comparison to a conventional Pt/SiO2 catalyst showed very similar activation energy, with E-app = 50 +/- 3 kJ.mol(-1). However, the turnover frequency over Pt/SiO2 was significantly lower, and Pt/SiO2 did not yield methane as a product. The Pt-containing UiO-67 Zr-MOF catalyst showed stable activity during 60 h of testing.
2017
56
45
13206
13218
http://pubs.acs.org/doi/10.1021/acs.iecr.7b01457
CO2 hydrogenation, Metal-organic Framework, Pt-functionalized UiO-67, metal nanoparticles, XRD, N2 adsorption, FESEM, TEM, Pt L3-edge XAS, dissolution-NMR, CO chemisorption, IR spectroscopy, TGA, catalytic testing
Gutterød, Emil Sebastian; Ø ien-Ødegaard, Sigurd; Bossers, Koen; Nieuwelink, Anne-Eva; Manzoli, Maela; Braglia, Luca; Lazzarini, Andrea; Borfecchia, E...espandi
File in questo prodotto:
File Dimensione Formato  
2017_Gutterod_Co2hydr_PtUiO67_IndEnginChemRes_OA.pdf

Open Access dal 23/01/2019

Descrizione: Articolo principale open access
Tipo di file: POSTPRINT (VERSIONE FINALE DELL’AUTORE)
Dimensione 2.59 MB
Formato Adobe PDF
2.59 MB Adobe PDF Visualizza/Apri
2017_Gutterod_Co2hydr_PtUiO67_IndEnginChemRes_edit.pdf

Accesso riservato

Descrizione: Articolo principale
Tipo di file: PDF EDITORIALE
Dimensione 2.47 MB
Formato Adobe PDF
2.47 MB Adobe PDF   Visualizza/Apri   Richiedi una copia

I documenti in IRIS sono protetti da copyright e tutti i diritti sono riservati, salvo diversa indicazione.

Utilizza questo identificativo per citare o creare un link a questo documento: https://hdl.handle.net/2318/1657661
Citazioni
  • ???jsp.display-item.citation.pmc??? ND
  • Scopus 66
  • ???jsp.display-item.citation.isi??? 65
social impact