1. XAS analysis of bifunctional Ni/ZSM-5 catalystsIztok Arčon, Hue-Tong Vu, Goran Dražić, Janez Volavšek, Gregor Mali, Nataša Zabukovec Logar, Nataša Novak Tušar, 2024, published scientific conference contribution abstract Abstract: In a bifunctional Ni/ZSM-5 zeolite type catalyst, catalytic properties are usually tuned via varying Al
and Ni contents [1]. Here we present a systematic structural study of the Ni/ZSM-5 materials by Ni
K-edge XANES and EXAFS analyses, to monitor the changes of local structure and chemical state
of Ni species in the catalysts as a function of Al and Ni content. A series of Ni/ZSM-5 type zeolites
with different Al to Si and Ni to Si molar ratios were synthesized by a “green”, template free technique
[2]. With a combination of XAS, XRD and TEM we resolved the changes in the local environment
of Ni species induced by the different Al contents in the
Ni/ZSM-5 catalysts.
Ni species in Ni/ZSM-5 exist as NiO nanocrystals and as
charge compensating Ni2+ cations. The Ni K-edge
XANES and EXAFS results enabled the quantification
of Ni-containing species. At a low Al to Si ratio (nAl/nSi
< 0.04), the NiO nanoparticles predominate in the
samples and account for over 65% of Ni phases.
However, NiO is outnumbered by Ni2+ cations attached
to the zeolite framework in ZSM-5 with a high Al to Si
ratio (nAl/nSi = 0.05) due to a higher number of
framework negative charges imparted by Al. The
obtained results show that the number of highly reducible
and active NiO nanocrystals is strongly correlated with
the framework Al sites present in Ni/ZSM-5 zeolites.
Keywords: Ni EXAFS, XANES Ni/ZSM-5 catalyst
Published in RUNG: 05.07.2024; Views: 572; Downloads: 3
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2. Efficient electrochemical nitrogen fixation at iron phosphide (Fe_2P) catalyst in alkaline mediumBeata Rytelewska, Anna Chmielnicka, Takwa Chouki, Magdalena Skunik-Nuckowka, Shaghayegh Naghdi, Dominik Eder, Aleksandra Michalowska, Tomasz Ratajczyk, Egon Pavlica, Saim Emin, 2023, original scientific article Abstract: A catalytic system based on iron phosphide (Fe2P) has exhibited electrocatalytic activity toward N2-reduction reaction in alkaline medium (0.5 mol dm−3 NaOH). Based on voltammetric stripping-type electroanalytical measurements, Raman spectroscopic and spectrophotometric data, it can be stated that the Fe2P catalyst facilitates conversion of N2 to NH3, and the process is fairly selective with respect to the competing hydrogen evolution. A series of diagnostic electrocatalytic experiments (utilizing platinum nanoparticles and HKUST-1) have been proposed and performed to control purity of nitrogen gas and to probe presence of potential contaminants such as ammonia, nitrogen oxo-species and oxygen. On the whole, the results are consistent with the view that the interfacial reduced-iron (Fe0) centers, while existing within the network of P sites, induce activation and reduction of nitrogen, parallel to the water splitting (reduction) to hydrogen. It is apparent from Tafel plots and impedance measurements that mechanism and dynamics of nitrogen reduction depends on the applied electroreduction potential. The catalytic system exhibits certain tolerance with respect to the competitive hydrogen evolution and gives (during electrolysis at -0.4 V vs. RHE) the Faradaic efficiency, namely, the selectivity (molar) efficiency, toward production of NH3 on the level of 60%. Under such conditions, the NH3-yield rate has been found to be equal to 7.5 µmol cm−2 h−1 (21 µmol m−2 s−1). By referring to classic concepts of electrochemical kinetic analysis, the rate constant in heterogeneous units has been found to be on the moderate level of 1-2*10−4 cm s−1 (at -0.4 V). The above mentioned iron-phosphorous active sites, which are generated on surfaces of Fe2P particles, have also been demonstrated to exhibit strong catalytic properties during reductions of other electrochemically inert reactants, such as oxygen, nitrites and nitrates.
Keywords: nitrogen reduction, alkaline medium, iron phosphide catalyst, ammonia, electrochemical determinations
Published in RUNG: 30.11.2023; Views: 1397; Downloads: 5
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3. Self-adaptive amorphous ▫$CoO_xCl_y$▫ electrocatalyst for sustainable chlorine evolution in acidic brineMengjun Xiao, Qianbao Wu, Ruiqi Ku, Liujiang Zhou, Chang Long, Junwu Liang, Andraž Mavrič, Lei Li, Jing Zhu, Matjaž Valant, 2023, original scientific article Abstract: Electrochemical chlorine evolution reaction is of central importance in the chlor-alkali industry, but the chlorine evolution anode is largely limited by water oxidation side reaction and corrosion-induced performance decay in strong acids. Here we present an amorphous CoOxCly catalyst that has been deposited in situ in an acidic saline electrolyte containing Co2+ and Cl- ions to adapt to the given electrochemical condition and exhibits ~100% chlorine evolution selectivity with an overpotential of ~0.1 V at 10 mA cm−2 and high stability over 500 h. In situ spectroscopic studies and theoretical calculations reveal that the electrochemical introduction of Cl- prevents the Co sites from charging to a higher oxidation state thus suppressing the O-O bond formation for oxygen evolution. Consequently, the chlorine evolution selectivity has been enhanced on the Cl-constrained Co-O* sites via the Volmer-Heyrovsky pathway. This study provides fundamental insights into how the reactant Cl-itself can work as a promoter toward enhancing chlorine evolution in acidic brine.
Keywords: catalyst synthesis, electrocatalysis, chlorine evolution
Published in RUNG: 04.09.2023; Views: 1864; Downloads: 8
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4. Multicomponent Cu-Mn-Fe silica supported catalysts to stimulate photo-Fenton-like water treatment under sunlightAndraž Šuligoj, Ivalina Trendafilova, Ksenija Maver, Albin Pintar, Alenka Ristić, Goran Dražić, Wael H. M. Abdelraheem, Zvonko Jagličić, Iztok Arčon, Nataša Zabukovec Logar, Dionysios D. Dionysiou, Nataša Novak Tušar, original scientific article Keywords: Magnetic catalyst, Photocatalyst, Water treatment, Sunlight, Contaminants of emerging concern, Photo-Fenton-like systems, Cu, Mn, Fe, XANES, EXAFS
Published in RUNG: 06.07.2023; Views: 2102; Downloads: 9
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5. Efficient Iron Phosphide Catalyst as a Counter Electrode in Dye-Sensitized Solar Cells : articleAbdullah Yildiz, Takwa Chouki, Aycan Atli, Moussab Harb, Sammy W Verbruggen, Rajeshreddy Ninakanti, Saim Emin, 2021, original scientific article Abstract: Developing an efficient material as a counter electrode (CE) with excellent catalytic activity, intrinsic stability, and low cost is essential for the commercial application of dye-sensitized solar cells (DSSCs). Transition metal phosphides have been demonstrated as outstanding multifunctional catalysts in a broad range of energy conversion technologies. Here, we exploited different phases of iron phosphide as CEs in DSSCs with an I–/I3–-based electrolyte. Solvothermal synthesis using a triphenylphosphine precursor as a phosphorus source allows to grow a Fe2P phase at 300 °C and a FeP phase at 350 °C. The obtained iron phosphide catalysts were coated on fluorine-doped tin oxide substrates and heat-treated at 450 °C under an inert gas atmosphere. The solar-to-current conversion efficiency of the solar cells assembled with the Fe2P material reached 3.96 ± 0.06%, which is comparable to the device assembled with a platinum (Pt) CE. DFT calculations support the experimental observations and explain the fundamental origin behind the improved performance of Fe2P compared to FeP. These results indicate that the Fe2P catalyst exhibits excellent performance along with desired stability to be deployed as an efficient Pt-free alternative in DSSCs.
Keywords: Iron phosphide, catalyst, counter electrode, dye-sensitized solar cell, solvothermal synthesis
Published in RUNG: 06.02.2023; Views: 1634; Downloads: 0
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6. Progressive pedagogies for innovation among art, science and technology : the case of mastmodule.euPeter Purg, N. Castillo-Rutz, Sergi Bermúdez i Badia, C. Csíkszentmihályi, Jurij V. Krpan, F. Hedeer, D. L. Sousa, Klemen Širok, 2022, original scientific article Abstract: Even if aiming at technical innovation, an interdisciplinary curriculum can and should include social
values. The Master Module in Art, Science and Technology project attempted to do so by developing
the innovation catalyst profile, a graduate who critically reflects on the creation process by combining
art thinking and design thinking. Within a pilot of the MAST module students from three universities
responded to timely challenges such as ‘The Future of Work’ and ‘Solidarity,’ through which the project
staff tested progressive pedagogical solutions like cross-disciplinary mentoring and situated knowledge
sharing. Introducing European social values in both artistic and technical education, the article presents
models, experiments and inspirations discussed against discursive analysis and course evaluation data.
In order to support not only inclusive but also sustainable teaching and learning approaches, novel
methods and tools may become daringly innovative as well as critical of both their pedagogical and
the wider social setting.
Keywords: art thinking, curriculum design, social values, innovation catalyst, design thinking
Published in RUNG: 27.06.2022; Views: 2241; Downloads: 30
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7. 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 ReactionMaja Pori, Iztok Arčon, Venkata Dasireddy, Blaž Likozar, 2021, original scientific article Abstract: 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.
Keywords: CH3OH synthesis, Cu/ZnO-based catalyst, XPS, XANES, EXAFS analyses, Catalyst selectivity and activity
Published in RUNG: 03.06.2021; Views: 2901; Downloads: 0
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8. Effect of the Morphology of the High-Surface-Area Support on the Performance of the Oxygen-Evolution Reaction for Iridium NanoparticlesLeonard Moriau, Marjan Bele, Živa Marinko, Francisco Ruiz-Zepeda, Gorazd Koderman, Martin Šala, Angelija Kjara Šurca, Janez Kovač, Iztok Arčon, Primož Jovanovič, Nejc Hodnik, Luka Suhadolnik, 2021, original scientific article Abstract: The development of affordable, low-iridium-loading,
scalable, active, and stable catalysts for the oxygen-evolution
reaction (OER) is a requirement for the commercialization of
proton-exchange membrane water electrolyzers (PEMWEs).
However, the synthesis of high-performance OER catalysts with
minimal use of the rare and expensive element Ir is very challenging
and requires the identification of electrically conductive and stable
high-surface-area support materials. We developed a synthesis
procedure for the production of large quantities of a nanocomposite
powder containing titanium oxynitride (TiONx) and Ir.
The catalysts were synthesized with an anodic oxidation process
followed by detachment, milling, thermal treatment, and the
deposition of Ir nanoparticles. The anodization time was varied to grow three different types of nanotubular structures exhibiting different lengths and wall thicknesses and thus a variety of properties. A comparison of milled samples with different degrees of nanotubular clustering and morphology retention, but with identical
chemical compositions and Ir nanoparticle size distributions and dispersions, revealed that the nanotubular support morphology is
the determining factor governing the catalyst’s OER activity and stability. Our study is supported by various state-of-the-art
materials’ characterization techniques, like X-ray photoelectron spectroscopy, scanning and transmission electron microscopies, Xray powder diffraction and absorption spectroscopy, and electrochemical cyclic voltammetry. Anodic oxidation proved to be a very suitable way to produce high-surface-area powder-type catalysts as the produced material greatly outperformed the IrO2 benchmarks
as well as the Ir-supported samples on morphologically different TiONx from previous studies. The highest activity was achieved for the sample prepared with 3 h of anodization, which had the most appropriate morphology for the effective removal of oxygen
bubbles.
Keywords: electrocatalysis, oxygen-evolution reaction, TiONx-Ir powder catalyst, iridium nanoparticles, anodic oxidation, morphology−activity correlation
Published in RUNG: 04.01.2021; Views: 3130; Downloads: 0
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9. Designing new renewable nano-structured electrode and membrane materials for direct alkaline ethanol fuel cell : Information on catalytic activity, structure and electric current con- ductivity of new catalysts on supporting substratesEgon Pavlica, Gvido Bratina, Jørgen Svendby, Qingjun Chen, Jia Yang, De Chen, Ji-Song Huang, Jessie Lue Shingjiang, 2020, final research report Keywords: fuel cell, ethanol oxidation, graphene, oxygen reduction, catalyst, pt-free, electrochemical impedance spectroscopy
Published in RUNG: 03.12.2020; Views: 3527; Downloads: 0
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