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25. Water Adsorption and Dissociation on Polycrystalline Copper Oxides: Effects of Environmental Contamination and Experimental Protocol

Author

Trotochaud, Lena, Head, Ashley R, Pletincx, Sven, Karslıoǧlu, Osman, Yu, Yi, Waldner, Astrid, Kyhl, Line, Hauffman, Tom, Terryn, Herman, Eichhorn, Bryan, and Bluhm, Hendrik

Subjects
Physical Sciences, Chemical Sciences, Physical Chemistry, Engineering, Chemical sciences, Physical sciences
Abstract

We use ambient-pressure X-ray photoelectron spectroscopy (APXPS) to study chemical changes, including hydroxylation and water adsorption, at copper oxide surfaces from ultrahigh vacuum to ambient relative humidities of ∼5%. Polycrystalline CuO and Cu2O surfaces were prepared by selective oxidation of metallic copper foils. For both oxides, hydroxylation occurs readily, even at high-vacuum conditions. Hydroxylation on both oxides plateaus near ∼0.01% relative humidity (RH) at a coverage of ∼1 monolayer. In contrast to previous studies, neither oxide shows significant accumulation of molecular water; rather, both surfaces show a high affinity for adventitious carbon contaminants. Results of isobaric and isothermic experiments are compared, and the strengths and potential drawbacks of each method are discussed. We also provide critical evaluations of the effects of the hot filament of the ion pressure gauge on the reactivity of gas-phase species, the peak fitting procedure on the quantitative analysis of spectra, and rigorous accounting of carbon contamination on data analysis and interpretation. This work underscores the importance of considering experimental design and data analysis protocols during APXPS experiments with water vapor in order to minimize misinterpretations arising from these factors.

Published
2018

27. Advancing Surgical Arrhythmia Ablation: Novel Insights on 3D Printing Applications and Two Biocompatible Materials

Author

Monaco, Cinzia, primary, Kronenberger, Rani, additional, Talevi, Giacomo, additional, Pannone, Luigi, additional, Cappello, Ida Anna, additional, Candelari, Mara, additional, Ramak, Robbert, additional, Della Rocca, Domenico Giovanni, additional, Bori, Edoardo, additional, Terryn, Herman, additional, Baert, Kitty, additional, Laha, Priya, additional, Krasniqi, Ahmet, additional, Gharaviri, Ali, additional, Bala, Gezim, additional, Chierchia, Gian Battista, additional, La Meir, Mark, additional, Innocenti, Bernardo, additional, and de Asmundis, Carlo, additional

Published
2024
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32. Synthesis and texturization processes of (super)-hydrophobic fluorinated surfaces by atmospheric plasma

Author

Hubert, Julie, Mertens, Jérémy, Dufour, Thierry, Vandencasteele, Nicolas, Reniers, François, Viville, Pascal, Lazzaroni, Roberto, Raes, M, and Terryn, Herman

Subjects
Physics - Plasma Physics
Abstract

The synthesis and texturization processes of fluorinated surfaces by means of atmospheric plasma are investigated and presented through an integrated study of both the plasma phase and the resulting material surface. Three methods enhancing the surface hydrophobicity up to the production of super-hydrophobic surfaces are evaluated: (i) the modification of a polytetrafluoroethylene (PTFE) surface, (ii) the plasma deposition of fluorinated coatings and (iii) the incorporation of nanoparticles into those fluorinated films. In all the approaches, the nature of the plasma gas appears to be a crucial parameter for the desired property. Although a higher etching of the PTFE surface can be obtained with a pure helium plasma, the texturization can only be created if O2 is added to the plasma, which simultaneously decreases the total etching. The deposition of CxFy films by a dielectric barrier discharge leads to hydrophobic coatings with water contact angles (WCAs) of 115{\textdegree}, but only the filamentary argon discharge induces higher WCAs. Finally, nanoparticles were deposited under the fluorinated layer to increase the surface roughness and therefore produce super-hydrophobic hybrid coatings characterized by the nonadherence of the water droplet at the surface., Comment: arXiv admin note: text overlap with arXiv:1604.08801

Published
2016
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37. Unravelling the Chemical Influence of Water on the PMMA/Aluminum Oxide Hybrid Interface In Situ.

Author

Pletincx, Sven, Marcoen, Kristof, Trotochaud, Lena, Fockaert, Laura-Lynn, Mol, Johannes MC, Head, Ashley R, Karslioğlu, Osman, Bluhm, Hendrik, Terryn, Herman, and Hauffman, Tom

Subjects
Biochemistry and Cell Biology, Other Physical Sciences
Abstract

Understanding the stability of chemical interactions at the polymer/metal oxide interface under humid conditions is vital to understand the long-term durability of hybrid systems. Therefore, the interface of ultrathin PMMA films on native aluminum oxide, deposited by reactive adsorption, was studied. The characterization of the interface of the coated substrates was performed using ambient pressure X-ray photoelectron spectroscopy (APXPS), Fourier transform infrared spectroscopy in the Kretschmann geometry (ATR-FTIR Kretschmann) and time-of-flight secondary ion mass spectrometry (ToF-SIMS). The formation of hydrogen bonds and carboxylate ionic bonds at the interface are observed. The formed ionic bond is stable up to 5 Torr water vapour pressure as shown by APXPS. However, when the coated samples are exposed to an excess of aqueous electrolyte, an increase in the amount of carboxylate bonds at the interface, as a result of hydrolysis of the methoxy group, is observed by ATR-FTIR Kretschmann. These observations, supported by ToF-SIMS spectra, lead to the proposal of an adsorption mechanism of PMMA on aluminum oxide, which shows the formation of methanol at the interface and the effect of water molecules on the different interfacial interactions.

Published
2017

38. In Situ Characterization of the Initial Effect of Water on Molecular Interactions at the Interface of Organic/Inorganic Hybrid Systems.

Author

Pletincx, Sven, Trotochaud, Lena, Fockaert, Laura-Lynn, Mol, Johannes MC, Head, Ashley R, Karslıoğlu, Osman, Bluhm, Hendrik, Terryn, Herman, and Hauffman, Tom

Subjects
Biochemistry and Cell Biology, Other Physical Sciences
Abstract

Probing initial interactions at the interface of hybrid systems under humid conditions has the potential to reveal the local chemical environment at solid/solid interfaces under real-world, technologically relevant conditions. Here, we show that ambient pressure X-ray photoelectron spectroscopy (APXPS) with a conventional X-ray source can be used to study the effects of water exposure on the interaction of a nanometer-thin polyacrylic acid (PAA) layer with a native aluminum oxide surface. The formation of a carboxylate ionic bond at the interface is characterized both with APXPS and in situ attenuated total reflectance Fourier transform infrared spectroscopy in the Kretschmann geometry (ATR-FTIR Kretschmann). When water is dosed in the APXPS chamber up to 5 Torr (~28% relative humidity), an increase in the amount of ionic bonds at the interface is observed. To confirm our APXPS interpretation, complementary ATR-FTIR Kretschmann experiments on a similar model system, which is exposed to an aqueous electrolyte, are conducted. These spectra demonstrate that water leads to an increased wet adhesion through increased ionic bond formation.

Published
2017

43. Advancing Surgical Arrhythmia Ablation: Novel Insights on 3D Printing Applications and Two Biocompatible Materials

Author

Monaco, Cinzia, Kronenberger, Rani, Talevi, Giacomo, Pannone, Luigi, Cappello, Ida Anna, Candelari, Mara, Ramak, Robbert, Della Rocca, Domenico Giovanni, Bori, Edoardo, Terryn, Herman, Baert, Kitty, Laha, Priya, Krasniqi, Ahmet, Gharaviri, Ali, Bala, Gezim, Chierchia, Gian-Battista, Meir, Mark La, Innocenti, Bernardo, de Asmundis, Carlo, Monaco, Cinzia, Kronenberger, Rani, Talevi, Giacomo, Pannone, Luigi, Cappello, Ida Anna, Candelari, Mara, Ramak, Robbert, Della Rocca, Domenico Giovanni, Bori, Edoardo, Terryn, Herman, Baert, Kitty, Laha, Priya, Krasniqi, Ahmet, Gharaviri, Ali, Bala, Gezim, Chierchia, Gian-Battista, Meir, Mark La, Innocenti, Bernardo, and de Asmundis, Carlo

Abstract

To date, studies assessing the safety profile of 3D printing materials for application in cardiac ablation are sparse. Our aim is to evaluate the safety and feasibility of two biocompatible 3D printing materials, investigating their potential use for intra-procedural guides to navigate surgical cardiac arrhythmia ablation. Herein, we 3D printed various prototypes in varying thicknesses (0.8 mm–3 mm) using a resin (MED625FLX) and a thermoplastic polyurethane elastomer (TPU95A). Geometrical testing was performed to assess the material properties pre- and post-sterilization. Furthermore, we investigated the thermal propagation behavior beneath the 3D printing materials during cryo-energy and radiofrequency ablation using an in vitro wet-lab setup. Moreover, electron microscopy and Raman spectroscopy were performed on biological tissue that had been exposed to the 3D printing materials to assess microparticle release. Post-sterilization assessments revealed that MED625FLX at thicknesses of 1 mm, 2.5 mm, and 3 mm, along with TPU95A at 1 mm and 2.5 mm, maintained geometrical integrity. Thermal analysis revealed that material type, energy source, and their factorial combination with distance from the energy source significantly influenced the temperatures beneath the 3D-printed material. Electron microscopy revealed traces of nitrogen and sulfur underneath the MED625FLX prints (1 mm, 2.5 mm) after cryo-ablation exposure. The other samples were uncontaminated. While Raman spectroscopy did not detect material release, further research is warranted to better understand these findings for application in clinical settings., SCOPUS: ar.j, info:eu-repo/semantics/published

Published
2024

44. Effect of Impregnation of PEDOT:PSS in Etched Aluminium Electrodes on the Performance of Solid State Electrolytic Capacitors.

Author

Calabia Gascón, Néstor, Wouters, Benny, Terryn, Herman, and Hubin, Annick

Subjects
ALUMINUM electrodes, ELECTRODE performance, ELECTROLYTIC capacitors, POROUS electrodes, MANUFACTURING processes
Abstract

Electrolytic capacitors store larger amounts of energy thanks to their thin dielectric layers and enlarged surface area. However, the benefits of using a liquid electrolyte are at the expense of the possibility of leakage, evaporation, or rupture of the device over time. As a solution, solid electrolytes, such as conductive polymers, substitute the liquid ones decreasing the internal resistance and enlarging the lifetime of these devices. PEDOT:PSS is a widely used conductive polymer in the formation of solid electrolytic capacitors. However, using the enlarged surface of the porous electrodes efficiently requires industrial processes, the efficacy of which has not been explored. In this work, porous aluminium electrodes with dielectric layers of different thicknesses were coated with PEDOT:PSS at different levels of doping in order to study the efficiency of the production of solid electrolytic capacitors in industry. The combination of odd random phase electrochemical impedance spectroscopy (ORP-EIS) with surface characterization techniques (SEM-EDX, GDOES) formed a methodology that allowed the study of both the electrical properties and the level of impregnation for these model systems. All samples consisting of a porous aluminium electrode with an amount of PEDOT:PSS deposited on top resulted in an inefficient degree of penetration between the two electrodes. However, the electrochemical analysis proved that the use of dopants produces systems with the highest capacitive properties. Consequently, the evolution towards better solid electrolytic capacitors does not rely solely on the proper coverage of the porous electrodes, but on the proper electrical properties of the PEDOT:PSS within the pores. [ABSTRACT FROM AUTHOR]

Published
2024
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