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1.
XAS analysis of bifunctional Ni/ZSM-5 catalysts
Iztok Arčon, Hue-Tong Vu, Goran Dražić, Janez Volavšek, Gregor Mali, Nataša Zabukovec Logar, Nataša Novak Tušar, 2024, objavljeni povzetek znanstvenega prispevka na konferenci

Opis: 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.
Ključne besede: Ni EXAFS, XANES Ni/ZSM-5 catalyst
Objavljeno v RUNG: 05.07.2024; Ogledov: 191; Prenosov: 1
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2.
Insight into the interdependence of Ni and Al in bifunctional Ni/ZSM-5 catalysts by Ni K-edge XAS analysis
Iztok Arčon, Hue-Tong Vu, Goran Dražić, Janez Volavšek, Gregor Mali, Nataša Zabukovec Logar, Nataša Novak Tušar, 2023, objavljeni povzetek znanstvenega prispevka na konferenci

Opis: Catalyst design is crucial for improving catalytic activity and product selectivity. In a bifunctional Ni/ZSM-5 zeolite type catalyst, catalytic properties are usually tuned via varying Al and Ni contents [1]. While changes in acid properties associated with Al sites are usually closely investigated, Ni phases, however, receive inadequate attention. Herein, we present a systematic structural study of Ni in the Ni/ZSM-5 materials by Ni K-edge XANES (X-ray absorption near edge structure) and EXAFS (extended X-ray absorption fine structure) analyses, to monitor the local structure and chemical state of Ni species in the catalysts. In combination with XRD and TEM we resolved the changes in the local environment of Ni species induced by the different Al contents of the parent ZSM-5 prepared by a “green”, template free technique [2]. Ni species in Ni/ZSM-5 exist as NiO crystals (3–50 nm) and as charge compensating Ni2+ cations. The Ni Kedge 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 crystals is strongly correlated with the framework Al sites present in ZSM-5 zeolites, which depend greatly on the synthesis conditions. Therefore, this kind of study is beneficial for any further investigation of the catalytic activities of Ni/ZSM-5 and other metal-modified bifunctional catalysts.
Ključne besede: Ni/ZSM-5 catalysts, Ni EXAFS, XANES
Objavljeno v RUNG: 19.09.2023; Ogledov: 1121; Prenosov: 3
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3.
In vitro tumor hypoxia imaging with fluorescent covalent organic frameworks
Tina Skorjanc, Dinesh Shetty, Damjan Makuc, Gregor Mali, Martina Bergant Marušič, Matjaž Valant, 2023, objavljeni povzetek znanstvenega prispevka na konferenci

Opis: Hypoxia refers to a condition where cells and tissues experience low, inadequate levels of O2. While healthy tissues are typically supplied with sufficient O2 (normoxia), cancerous tissues commonly face hypoxia due to the tumor’s extraordinarily high demand for oxygen. Various fluorescent small-molecule probes have been designed for selective detection of hypoxia in living cells, but few nanomaterials have been investigated for this type of bioimaging. Herein, we prepare a fluorescent covalent organic framework (COF) with β-ketoenamine linkages and post-synthetically modify it to conjugate hypoxia-sensitive nitroimidazole moieties into its pores (NI-COF). Stacks of sheets in NI-COF observed under electron microscopy were exfoliated by ultrasonication, and dynamic light scattering measurements confirmed particle size of less than 200 nm. Thus-prepared material exhibited good stability in physiological conditions and low cytotoxicity in in vitro experiments. NI-COF also showed useful fluorescence properties with an emission peak at 490 nm (λex = 420 nm) at both neutral and mildly acidic pH levels that are characteristic of tumor tissues. Encouraged by the favorable properties of the material, we incubated HeLa cells pre-treated in either hypoxic or normoxic conditions with NI-COF. Fluorescence microscopy images demonstrated that the material was preferentially taken up by hypoxic cells, which showed higher fluorescence signal in their interior than cells cultured under normoxia conditions. It is anticipated that this study will stimulate further developments of COFs for imaging various biological conditions.
Ključne besede: hypoxia, fluorescence, covalent organic frameworks, imaging, tumor cells
Objavljeno v RUNG: 19.09.2023; Ogledov: 1127; Prenosov: 4
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4.
Winning combination of Cu and Fe oxide clusters with an alumina support for low-temperature catalytic oxidation of volatile organic compounds
Tadej Žumbar, Iztok Arčon, Petar Djinović, Giuliana Aquilanti, Gregor Žerjav, Albin Pintar, Alenka Ristić, Goran Dražić, Janez Volavšek, Gregor Mali, Margarita Popova, Nataša Zabukovec Logar, Nataša Novak Tušar, 2023, izvirni znanstveni članek

Opis: A γ-alumina support functionalized with transition metals is one of the most widely used industrial catalysts for the total oxidation of volatile organic compounds (VOCs) as air pollutants at higher temperatures (280−450 °C). By rational design of a bimetal CuFe-γ-alumina catalyst, synthesized from a dawsonite alumina precursor, the activity in total oxidation of toluene as a model VOC at a lower temperature (200−380 °C) is achieved. A fundamental understanding of the catalyst and the reaction mechanism is elucidated by advanced microscopic and spectroscopic characterizations as well as by temperature-programmed surface techniques. The nature of the metal−support bonding and the optimal abundance between Cu−O−Al and Fe−O−Al species in the catalysts leads to synergistic catalytic activity promoted by small amounts of iron (Fe/Al = 0.005). The change in the metal oxide−cluster alumina interface is related to the nature of the surfaces to which the Cu atoms attach. In the most active catalyst, the CuO6 octahedra are attached to 4 Al atoms, while in the less active catalyst, they are attached to only 3 Al atoms. The oxidation of toluene occurs via the Langmuir−Hinshelwood mechanism. The presented material introduces a prospective family of low-cost and scalable oxidation catalysts with superior efficiency at lower temperatures.
Ključne besede: Iron oxide clusters, copper oxide clusters, alumina support, synergistic effect, low-temperature total catalytic oxidation, toluene, Cu, Fe XANES, EXAFS
Objavljeno v RUNG: 06.07.2023; Ogledov: 1534; Prenosov: 15
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5.
Covalent organic frameworks for fluorescent imaging of hypoxia
Tina Škorjanc, Dinesh Shetty, Gregor Mali, Damjan Makuc, Martina Bergant Marušič, Matjaž Valant, 2023, objavljeni povzetek znanstvenega prispevka na konferenci

Ključne besede: hypoxia, covalent organic frameworks, imaging, fluorescence, post-synthetic modification
Objavljeno v RUNG: 06.06.2023; Ogledov: 1394; Prenosov: 2
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Covalent polymer thin films for biosensor applications
Tina Skorjanc, Andraž Mavrič, Mads Nybo Sorensen, Gregor Mali, Changzhu Wu, Matjaž Valant, 2022, objavljeni povzetek znanstvenega prispevka na konferenci

Ključne besede: bacteria, sensing, electrochemical impedance spectroscopy, electrophoresis, electrode preparation, Menshutkin reaction
Objavljeno v RUNG: 26.09.2022; Ogledov: 1500; Prenosov: 0
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