7 results
Search Results
Now showing 1 - 7 of 7
- ItemRole of Reaction Intermediate Diffusion on the Performance of Platinum Electrodes in Solid Acid Fuel Cells(Basel : MDPI, 2021) Lorenz, Oliver; Kühne, Alexander; Rudolph, Martin; Diyatmika, Wahyu; Prager, Andrea; Gerlach, Jürgen W.; Griebel, Jan; Winkler, Sara; Lotnyk, Andriy; Anders, André; Abel, BerndUnderstanding the reaction pathways for the hydrogen oxidation reaction (HOR) and the oxygen reduction reaction (ORR) is the key to design electrodes for solid acid fuel cells (SAFCs). In general, electrochemical reactions of a fuel cell are considered to occur at the triple-phase boundary where an electrocatalyst, electrolyte and gas phase are in contact. In this concept, diffusion processes of reaction intermediates from the catalyst to the electrolyte remain unconsidered. Here, we unravel the reaction pathways for open-structured Pt electrodes with various electrode thicknesses from 15 to 240 nm. These electrodes are characterized by a triple-phase boundary length and a thickness-depending double-phase boundary area. We reveal that the double-phase boundary is the active catalytic interface for the HOR. For Pt layers ≤ 60 nm, the HOR rate is rate-limited by the processes at the gas/catalyst and/or the catalyst/electrolyte interface while the hydrogen surface diffusion step is fast. For thicker layers (>60 nm), the diffusion of reaction intermediates on the surface of Pt be-comes the limiting process. For the ORR, the predominant reaction pathway is via the triple-phase boundary. The double-phase boundary contributes additionally with a diffusion length of a few nanometers. Based on our results, we propose that the molecular reaction mechanism at the electrode interfaces based upon the triple-phase boundary concept may need to be extended to an effective area near the triple-phase boundary length to include all catalytically relevant diffusion processes of the reaction intermediates. © 2021 by the authors. Licensee MDPI, Basel, Switzerland.
- ItemTime-resolved ion energy and charge state distributions in pulsed cathodic arc plasmas of Nb−Al cathodes in high vacuum(Bristol : IOP Publ., 2018-5-15) Zöhrer, Siegfried; Anders, André; Franz, RobertCathodic arcs have been utilized in various applications including the deposition of thin films and coatings, ion implantation, and high current switching. Despite substantial progress in recent decades, the physical mechanisms responsible for the observed plasma properties are still a matter of dispute, particularly for multi-element cathodes, which can play an essential role in applications. The analysis of plasma properties is complicated by the generally occurring neutral background of metal atoms, which perturbs initial ion properties. By using a time-resolved method in combination with pulsed arcs and a comprehensive Nb−Al cathode model system, we investigate the influence of cathode composition on the plasma, while making the influence of neutrals visible for the observed time frame. The results visualize ion detections of 600 μs plasma pulses, extracted 0.27 m from the cathode, resolved in mass-per-charge, energy-per-charge and time. Ion properties are found to be strongly dependent on the cathode material in a way that cannot be deduced by simple linear extrapolation. Subsequently, current hypotheses in cathodic arc physics applying to multi-element cathodes, like the so-called 'velocity rule' or the 'cohesive energy rule', are tested for early and late stages of the pulse. Apart from their fundamental character, the findings could be useful in optimizing or designing plasma properties for applications, by actively utilizing effects on ion distributions caused by composite cathode materials and charge exchange with neutrals.
- ItemLow-temperature atmospheric pressure plasma conversion of polydimethylsiloxane and polysilazane precursor layers to oxide thin films(Weinheim : Wiley VCH, 2023) Rudolph, Martin; Birtel, Peter; Arnold, Thomas; Prager, Andrea; Naumov, Sergej; Helmstedt, Ulrike; Anders, André; With, Patrick C.We study the conversion of two polymeric silicon precursor compound layers (perhydropolysilazane and polydimethylsiloxane) on a silicon wafer and polyethylene terephthalate substrates to silicon oxide thin films using a pulsed atmospheric pressure plasma jet. Varying the scan velocity and the number of treatments results in various film compositions, as determined by X-ray photoelectron spectroscopy and Fourier transform infrared spectroscopy. The mechanism suggested for the conversion process includes the decomposition of the precursor triggered by plasma-produced species, the oxidation of the surface, and finally, the diffusion of oxygen into the film, while gases produced during the precursor decomposition diffuse out of the film. The latter process is possibly facilitated by local plasma heating of the surface. The precursor conversion appears to depend sensitively on the balance between the different contributions to the conversion mechanism.
- ItemInsights into surface modification and erosion of multi-element arc cathodes using a novel multilayer cathode design(Melville, NY : American Inst. of Physics, 2020) Golizadeh, Mehran; Anders, André; Martin, Francisca Mendez; Kolozsvári, Szilard; Franz, RobertNowadays, multi-element cathodes are frequently employed to grow multi-element thin films and coatings using cathodic arc deposition processes. During cathode erosion, the cathode spot sequentially ignites on the cathode surface and imposes melting-solidification cycles that lead to material intermixing and the formation of a modified layer on the cathode surface. To allow us to study these surface modifications, a 10 µm thick Mo/Al multilayer coating was sputter-deposited onto a standard Ti arc cathode. This cathode was eroded by a dc steered arc discharge for a short duration enabling the observation of single craters formed by type 1 and 2 cathode spots. Furthermore, separated clusters of overlapping craters and a fully eroded surface caused by different stages of erosion were differentiated when scanning the erosion track in the lateral direction. Cross sections of single craters were prepared by focused ion beam techniques while metallographic methods were applied to obtain cross sections of overlapping craters and the modified layer. The layers of the multilayer coating acted as trace markers providing new insights into the material intermixing within craters, the material displacements during crater formation, the plasma pressure acting on the craters, and the temperature gradient (heat-affected zone) below the craters. The observations are discussed within the framework of established arc crater formation models. © 2020 Author(s).
- ItemInfluence of wavelength and accumulated fluence at picosecond laser-induced surface roughening of copper on secondary electron yield(Melville, NY : American Inst. of Physics, 2023) Bez, Elena; Himmerlich, Marcel; Lorenz, Pierre; Ehrhardt, Martin; Gunn, Aidan Graham; Pfeiffer, Stephan; Rimoldi, Martino; Taborelli, Mauro; Zimmer, Klaus; Chiggiato, Paolo; Anders, AndréUltrashort-pulse laser processing of copper is performed in air to reduce the secondary electron yield (SEY). By UV (355 nm), green (532 nm), and IR (1064 nm) laser-light induced surface modification, this study investigates the influence of the most relevant experimental parameters, such as laser power, scanning speed, and scanning line distance (represented as accumulated fluence) on the ablation depth, surface oxidation, topography, and ultimately on the SEY. Increasing the accumulated laser fluence results in a gradual change from a Cu 2 O to a CuO-dominated surface with deeper micrometer trenches, higher density of redeposited surface particles from the plasma phase, and a reduced SEY. While the surface modifications are less pronounced for IR radiation at low accumulated fluence (,1000 J/cm2 ), analogous results are obtained for all wavelengths when reaching the nonlinear absorption regime, for which the SEY maximum converges to 0.7. Furthermore, independent of the extent of the structural transformations, an electron-induced surface conditioning at 250 eV allows a reduction of the SEY maximum below unity at doses of 5×10 -4 C/mm2 . Consequently, optimization of processing parameters for application in particle accelerators can be obtained for a sufficiently low SEY at controlled ablation depth and surface particle density, which are factors that limit the surface impedance and the applicability of the material processing for ultrahigh vacuum systems. The relations between pro- cessing parameters and surface features will provide guidance in treating the surface of vacuum components, especially beam screens of selected magnets of the Large Hadron Collider or of future colliders.
- ItemInfluence of Ar gas pressure on ion energy and charge state distributions in pulsed cathodic arc plasmas from Nb-Al cathodes studied with high time resolution(Bristol : IOP Publ., 2019) Zöhrer, Siegfried; Anders, André; Franz, RobertFor cathodic arcs, the cathode material is one of the most important determinants of plasma properties. Consequently, the cathode material - plasma relationship is of special interest in related fundamental research as well as in applications like the synthesis of thin films and coatings. In the latter, the use of multi-element cathodes in inert as well as reactive gas atmospheres is common practice. To further improve the physical understanding of cathodic arcs in such settings, we analyze ions in pulsed cathodic arc plasmas from Nb, Al and two composite Nb-Al cathodes with high time-resolution using a mass-energy-analyzer. The experiments were conducted in Ar atmosphere at total pressures of 0.04, 0.20 and 0.40 Pa, and are compared to earlier results in high vacuum at 10-4. In addition to examining the influence of Ar on ion properties and their cathode material dependence, the results are used to discuss physical concepts in cathodic arcs, like the gas-dynamic expansion of the cathode spot plasma, or the influence of charge exchange collisions of ions with neutrals. While such inelastic collisions e.g. with Ar atoms cause a reduction of charge states to mainly Al+ and Nb2+ at the highest pressure, Ar atoms also seem to take part in near-cathode processes. Ar ions in different time and energy regimes up to 150 eV were observed and compared to Nb and Al ions, showing overlapping velocity distributions for Nb, Al and Ar+ ions, but also Ar2+ ions faster than other ion species. © 2018 IOP Publishing Ltd.
- ItemUnravelling the ion-energy-dependent structure evolution and its implications for the elastic properties of (V,Al)N thin films(Kidlington : Elsevier Science, 2021) Karimi Aghda, Soheil; Music, Denis; Unutulmazsoy, Yeliz; Sua, Heng Han; Mráz, Stanislav; Hans, Marcus; Primetzhofer, Daniel; Anders, André; Schneider, Jochen M.Ion irradiation-induced changes in the structure and mechanical properties of metastable cubic (V,Al)N deposited by reactive high power pulsed magnetron sputtering are systematically investigated by correlating experiments and theory in the ion kinetic energy (Ek) range from 4 to 154 eV. Increasing Ek results in film densification and the evolution from a columnar (111) oriented structure at Ek ≤ 24 eV to a fine-grained structure with (100) preferred orientation for Ek ≥ 104 eV. Furthermore, the compressive intrinsic stress increases by 336 % to -4.8 GPa as Ek is increased from 4 to 104 eV. Higher ion kinetic energy causes stress relaxation to -2.7 GPa at 154 eV. These ion irradiation-induced changes in the thin film stress state are in good agreement with density functional theory simulations. Furthermore, the measured elastic moduli of (V,Al)N thin films exhibit no significant dependence on Ek. The apparent independence of the elastic modulus on Ek can be rationalized by considering the concurrent and balancing effects of bombardment-induced formation of Frenkel pairs (causing a decrease in elastic modulus) and evolution of compressive intrinsic stress (causing an increase in elastic modulus). Hence, the evolution of the film stresses and mechanical properties can be understood based on the complex interplay of ion irradiation-induced defect generation and annihilation.