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Okolju prijazna sinteza metanola s hidrogeniranjem ogljikovega dioksida preko trikomponentnih katalizatorjev
Teja Cankar, 2017, diplomsko delo

Opis: Zaradi naraščanja koncentracije CO2 v ozračju in njenega negativnega vpliva na okolje, se išče načine, s katerimi bi to koncentracijo zmanjšali. Ena izmed možnosti je direktna hidrogenacija atmosferskega CO2 do metanola, s čimer bi CO2 uporabili kot surovino, hkrati pa pridobili metanol, ki je uporabna kemikalija. Ta proces zahteva uporabo učinkovitega in stabilnega katalizatorja ter optimalne reakcijske pogoje. V tem raziskovalnem delu smo s katalitičnimi testi proučevali vpliv reakcijskih pogojev, različnih komponent katalizatorja in sinteznih metod na učinkovitost katalizatorjev za sintezo metanola. Kot optimalna temperatura in tlak sta se izkazala območja od 220 do 240 °C in od 40 do 50 barov, kjer je reakcija dovolj hitra, hkrati pa še ni bistveno termodinamsko zavrta, in pride do zadostne količine sintetiziranega metanola. Kot najbolj učinkovito molsko razmerje plinov se je izkazalo H2 : CO2 = 3 : 1 in kot najbolj učinkovita plinska urna prostorska hitrost 6000 h-1. To sta pogoja, kjer je količina sintetiziranega metanola zadosti velika ob sprejemljivi porabi reaktantov. Kot najbolj učinkovit katalizator se je izkazal komercialno uporabljen HiFUEL®, dobre lastnosti pa sta pokazala tudi CuO/MgO/Al2O3 in CuO/ZnO/CeO2. CuO/MgO/Al2O3 katalizator je dobro aktiven v širšem temperaturnem območju (220–260 °C), njegova aktivnost je okoli 0,6 molCH3OH•l-1•h-1. Prednost CuO/ZnO/CeO2 katalizatorja pa je izredno visoka selektivnost, in sicer pri 220 °C približno 65 %.
Najdeno v: osebi
Ključne besede: hidrogenacija CO2, sinteza metanola, učinkovitost katalizatorjev, reakcijski pogoji, različna sestava katalizatorjev
Objavljeno: 17.11.2017; Ogledov: 4304; Prenosov: 194
.pdf Polno besedilo (5,84 MB)

Photo-Chemically-Deposited and Industrial Cu/ZnO/Al2O3 Catalyst Material Surface Structures During CO2 Hydrogenation to Methanol: EXAFS, XANES and XPS Analyses of Phases After Oxidation, Reduction, and Reaction
Blaž Likozar, Iztok Arčon, Venkata Dasireddy, Maja Pori, 2021, izvirni znanstveni članek

Opis: Industrial Cu/ZnO/Al2O3 or novel rate catalysts, prepared with a photochemical deposition method, were studied under functional CH3OH synthesis conditions at the set temperature (T) range of 240–350 °C, 20 bar pressure, and stoichiometric carbon dioxide/hydrogen composition. Analytical scanning electron microscopy (SEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), X-ray adsorption near edge structure (XANES) and extended X-ray absorption fine structure (EXAFS) methods were systematically utilized to investigate the interfaces, measured local geometry, and chemical state electronics around the structured active sites of commercially available Cu/ZnO/Al2O3 material or synthesized Cu/ZnO. Processed Cu K-edge EXAFS analysis suggested that various Cu atom species, clusters, metallic fcc Cu, Cu oxides (Cu2O or CuO) and the Cu0.7Zn2 alloy with hexagonal crystalline particles are contained after testing. It was proposed that in addition to the model’s Cu surface area, the amount, ratio and dispersion of the mentioned bonded Cu compounds significantly influenced activity. Additionally, XPS revealed that carbon may be deposited on the commercial Cu/ZnO/Al2O3, forming the inactive carbide coating with Cu or/and Zn, which may be the cause of basicity’s severe deactivation during reactions. The selectivity to methanol decreased with increasing T, whereas more Cu0.7Zn2 inhibited the CO formation through reverse water–gas shift (RWGS) CO2 reduction.
Najdeno v: osebi
Ključne besede: CH3OH synthesis, Cu/ZnO-based catalyst, XPS, XANES, EXAFS analyses, Catalyst selectivity and activity
Objavljeno: 03.06.2021; Ogledov: 1090; Prenosov: 0
.pdf Polno besedilo (3,98 MB)

Synthesis of a Cu/ZnO Nanocomposite by Electroless Plating for the Catalytic Conversion of CO2 to Methanol
Maja Pori, Iztok Arčon, Marjan Marinšek, Goran Dražić, Blaž Likozar, Zorica Crnjak Orel, Damjan Lašič Jurković, 2019, izvirni znanstveni članek

Opis: The process of methanol synthesis based on the hydrogenation of CO2 was investigated over binary Cu/ZnO catalyst materials, prepared by applying a novel electroless plating fabrication method. The activity of the produced catalytic samples was determined at temperature range between 200 and 300 °C and the feedstock conversion data were supplemented with a detailed microstructure analysis using high-resolution transmission electron microscopy (HRTEM), X-ray powder diffraction (XRD) and Cu and Zn K-edge, X-ray absorption near-edge structure (XANES) measurements and extended X-ray absorption fine-structure (EXAFS) measurements. It was confirmed that the disorder in the Cu crystallites created unique geometrical situations, which acted as the additional reactive centres for the adsorption of the reactant molecule species. Copper and zinc structural synergy (spill-over) was also demonstrated as being crucial for the carbon dioxide’s activation. EXAFS and XANES results provide strong evidence for surface alloying between copper and zinc and thus the present results demonstrate new approach applicable for explaining metal–support interactions.
Najdeno v: osebi
Ključne besede: EXAFS, CuZn alloy, Spillover mechanism, CO2 valorization, Electroless deposition method, Heterogeneous catalysis
Objavljeno: 12.04.2019; Ogledov: 2479; Prenosov: 0
.pdf Polno besedilo (1,92 MB)

Effect of Na, Cs and Ca on propylene epoxidation selectivity over CuOx/SiO2 catalysts studied by catalytic tests, in-situ XAS and DFT
Janvit Teržan, Matej Huš, Iztok Arčon, Blaž Likozar, Petar Djinović, 2020, izvirni znanstveni članek

Opis: This research focuses on epoxidation of propylene over pristine, Na, Ca and Cs modified CuOx/SiO2 catalysts using O2. The selectivity of the reaction is analyzed using a combination of catalytic tests, in-situ XAS and DFT calculations. The initially present subnanometer CuO clusters are present in all catalysts which re-disperse/flatten during reaction. During catalytic reaction, the Cu1+ becomes the predominant oxidation state. There is no correlation between propylene oxide (PO) selectivity and copper oxidation state. DFT analysis of the propylene reaction pathway revealed that Na, Cs, and Ca addition decreases the bonding strength of propylene to CuO and decreases the O2 activation barrier, while simultaneously increase the exothermicity of O2 dissociation. The Na induced Cu-O bond modification decreases the activation barrier from 0.87 to 0.71 eV for the oxametallacycle (OMC) ring closure (first step in the reaction pathway favoring selectivity towards PO) compared to pristine 5Cu catalyst. At the same time, we observed an increase (from 0.45 to 0.72 eV) of the barrier for the abstraction of allylic hydrogen. The opposite effect is achieved by Ca addition: the activation barrier for OMC ring closure increases to 1.08 eV and that for allylic hydrogen stripping decreases to 0.16 eV.
Najdeno v: osebi
Ključne besede: Alkali modification, propylene epoxidation, reaction mechanism, copper oxide, activation barrier.
Objavljeno: 05.06.2020; Ogledov: 1757; Prenosov: 0
.pdf Polno besedilo (22,78 MB)

CO[sub]2 activation over nanoshaped CeO[sub]2 decorated with nickel for low-temperature methane dry reforming
Kristijan Lorber, Janez Zavašnik, Iztok Arčon, Matej Huš, Janvit Teržan, Blaž Likozar, Petar Djinović, izvirni znanstveni članek

Opis: Dry reforming of methane (DRM) is a promising way to convert methane and carbon dioxide into H2 and CO (syngas). CeO2 nanorods, nanocubes, and nanospheres were decorated with 1−4 wt % Ni. The materials were structurally characterized using TEM and in situ XANES/EXAFS. The CO2 activation was analyzed by DFT and temperature-programmed techniques combined with MS-DRIFTS. Synthesized CeO2 morphologies expose {111} and {100} terminating facets, varying the strength of the CO2 interaction and redox properties, which influence the CO2 activation. Temperature-programmed CO2 DRIFTS analysis revealed that under hydrogen-lean conditions mono- and bidentate carbonates are hydrogenated to formate intermediates, which decompose to H2O and CO. In excess hydrogen, methane is the preferred reaction product. The CeO2 cubes favor the formation of a polydentate carbonate species, which is an inert spectator during DRM at 500 °C. Polydentate covers a considerable fraction of ceria’s surface, resulting in less-abundant surface sites for CO2 dissociation
Najdeno v: osebi
Ključne besede: surface carbonates, in situ characterization, Ni XANES, Ni EXAFS, spectator species, CeO2 nanoshapes, CO2 activation
Objavljeno: 13.07.2022; Ogledov: 246; Prenosov: 0
.pdf Polno besedilo (9,50 MB)

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