Faglige interesser
Zeolites, Zeotypes, Catalysis, Catalytic testing, Porous materials, Metal-Organic Frameworks, Methane-to-Methanol, CO2-hydrogenation, Chemical Industry, Material Science, Spectroscopy, Hydrocarbons
Bakgrunn
2018-2020
M.Sc. i Uorganisk kjemi og materialkjemi
Oppgaven: A Study of Catalytic Pt Nanoparticles inside a Nano-porous Functionalized UiO MOF-matrix for CO2-Hydrogenation
2015-2018
B.Sc. i Kjemi
Emneord:
Heterogeneous catalysis,
Testing,
Characterization,
SMN,
Katalyse,
iCSI
Publikasjoner
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Prodinger, Sebastian; Capel Berdiell, Izar; Cordero-Lanzac, Tomas; Bygdnes, Odd Reidar; Solemsli, Bjørn Gading & Kvande, Karoline
[Vis alle 10 forfattere av denne artikkelen]
(2023).
Cation-induced speciation of port-size during mordenite zeolite synthesis.
Journal of Materials Chemistry A.
ISSN 2050-7488.
11(40),
s. 21884–21894.
doi:
10.1039/d3ta03444e.
Fulltekst i vitenarkiv
Vis sammendrag
Mordenite (MOR) zeolite, an important industrial catalyst exists in two, isostructural variants defined by their port-size, small and large-port. Here we show for the first time how a systematic, single-parameter variation influences the synthesis out-come on the final MOR material leading to distinctly different catalysts. The cation identity has a direct impact on the synthesis mechanism with potassium cations generating the more constrained, small-port MOR variant compared to the large-port obtained with sodium cations. This was expressed by different degrees of accessibility ascertained with a combination of toluene breakthrough and temperature programmed desorption (TPD), propylamine TPD, as well as sterically sensitive isobutane conversion. Rietveld refinement of the X-ray diffractograms elucidated the preferential siting of the smaller sodium cations in the constricted 8-ring, from which differences in Al distribution follow. Note, there are no organic structure directing agents utilized in this synthesis pointing at the important role of inorganic structure directing agents (ISDA).
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Gutterød, Emil Sebastian; Pulumati, S.H.; Kaur, Gurpreet; Lazzarini, Andrea; Solemsli, Bjørn Garding & Gunnæs, Anette Eleonora
[Vis alle 13 forfattere av denne artikkelen]
(2020).
Influence of Defects and H2O on the Hydrogenation of CO2 to Methanol over Pt Nanoparticles in UiO-67 Metal-Organic Framework.
Journal of the American Chemical Society.
ISSN 0002-7863.
142(40),
s. 17105–17118.
doi:
10.1021/jacs.0c07153.
Fulltekst i vitenarkiv
Se alle arbeider i Cristin
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Kvande, Karoline; Prodinger, Sebastian; Borfecchia, Elisa; Garetto, Beatrice; Solemsli, Bjørn Gading & Signorile, Matteo
[Vis alle 10 forfattere av denne artikkelen]
(2022).
Structural and mechanistic investigations of CuxOy- sites in zeolites and their role in the direct activation of lower alkanes.
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Solemsli, Bjørn Gading; Kvande, Karoline; Prodinger, Sebastian & Svelle, Stian
(2022).
Fuels & Chemicals from Methane.
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Solemsli, Bjørn Gading; Svelle, Stian; Kvande, Karoline & Prodinger, Sebastian
(2022).
Direct Synthesis to Methanol from Methane over Cu-Zeolites
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Solemsli, Bjørn Gading; Svelle, Stian; Prodinger, Sebastian & Kvande, Karoline
(2022).
Methylation of Lower alkenes though stepwise reaction with methane.
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Solemsli, Bjørn Gading; Olsbye, Unni; Gunnæs, Anette Eleonora & Gutterød, Emil Sebastian
(2020).
A Study of Catalytic Pt Nanoparticles inside a Nano-porous Functionalized UiO MOF-matrix for CO2-Hydrogenation
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Universitetet i Oslo.
Vis sammendrag
Hydrogenation of carbon dioxide hasreceivedincreasingattentionin catalytic research the last decade as a sustainable alternativeforproducing high value chemicals thattodayare produced fromfossil fuels. The aim of this thesis has been two-fold: First, to study Pt nanoparticles formed in various UiO-66 and -67 metal-organic frameworks (MOFs) by Transmission Electron Microscopy (TEM), and second, to study the Pt-containing MOFs as catalysts for the CO2hydrogenation reaction.Three Zr-based UiO-66 MOF and nineUiO-67 MOF samples containing different amountsof functionalized linkers were impregnated withdifferent amounts ofK2PtCl4and reduced in H2at 350 ̊C for 4 hours to form Pt nanoparticles embedded in the MOF matrix.The samples were then testedin a H2/CO2feed at 8 bar and 170 ̊Cfor the hydrogenation reaction. After testing,TEMwas used to investigate the formation of Pt nanoparticles andtheir relationship with the surrounding MOF structure.
The study revealed that, despite variable the linkers in the MOF,the conversion of CO2isdominated bythe reverse water-gas shift reaction,suggestingthat the linkers donot partakethe reactions mechanisms. Analysis usingTEMrevealedthat the Pt nanoparticles grow independently of its surroundings inside the MOFs with no observable growth relationshipwith the MOF. The nanoparticles are seen to grow into octahedral crystals that are larger than the pores in the framework. Samples with different amountsof missing linker type defects show that the presence of open Zr-node sitesenhances the selectivity towards methanol. A sample of Pt-functionalized UiO-67 with 10% [2,2’-bipyridine]5,5’-dicaboxylicacidlinker was oxidised toinduce missing linkerdefects post synthetically. After reduction in H2at 350 ̊C for 4 hours, the sample was oxidized in situin synthetic air for three different time spans. Careful analysis with N2-adsroption and TEM revealedthat the structure of the MOF deteriorates and loses accessible surface area with increasing timeon steam, while keeping the dispersion of the Pt nanoparticles. PXRD analysis revealedthe formation of tetragonal ZrO2. Extensive testsfrom 1-30 bar and 170-375 ̊C reveal a lower conversion and higher selectivity towards methanol for a fully calcined sample, indicating that the Zr-nodes behave similarlyto non-MOF ZrO2supports. Transient kinetic studies of the parent UiO-67 sample revealedthat the sample behaves similarlytopreviously studied systemsby Gutterød et al., and showed the presence of an inverse kinetic isotope effect for methane and methanolformation upon H2/D2exchange.
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Publisert
18. feb. 2021 14:36
- Sist endret
20. sep. 2022 11:36