This dissertation aims to better understand the evolution of single hydrogen gas bubbles evolved during the water electrolysis at microelectrodes. In particular, the growth and detachment processes were studied in detail experimentally by means of electrochemical and optical methods in terrestrial, micro-, and hypergravity conditions. The combination of microelectrode and sulfuric acid promoting the bubble coalescence results in a periodical growth and the detachment of single bubbles. This provides a systematic view on the phenomena under study. A shadowgraphy system was used to provide general insight into the bubble behaviour, while Particle Tracking Velocimetry (PTV) was used for the flow velocity measurements around the growing hydrogen bubble. By applying high electric potentials considerably exceeding that in industrial electrolysers, it is possible to analyse the evolution of hydrogen bubbles under extreme conditions and for a wide range of electrolyte concentrations, overall shedding more light on bubble dynamics in general, and especially the underlying balance of forces.
The growth of single hydrogen bubbles at micro-electrodes was studied in an acidic electrolyte over a wide range of concentrations and cathodic potentials. New bubble growth regimes were identified which differ in terms of whether the bubble evolution proceeds in the presence of a monotonic or oscillatory variation in the electric current and a carpet of microbubbles underneath the bubble. Key features such as the growth law of the bubble radius, the dynamics of the microbubble carpet, the onset time of the oscillations and the oscillation frequencies were characterised as a function of the concentration and electric potential. Furthermore, the system's response to jumps in the cathodic potential was studied. The electrode, tilted to the horizon, promotes faster growth and, therefore, earlier detachment at the smaller volume of the bubble. During its evolution, the bubble moves laterally from the electrode centre, releasing the electrode area and enabling higher electric current, therefore faster hydrogen generation and bubble-bubble coalescence rates. The duration of the bubble position oscillations found on the horizontal electrode gradually reduces upon tilt angle increase, with an almost complete disappearance at 5°. Based on the analysis of the forces involved and their scaling with the concentration, potential and electric current, a sound hypothesis was formulated regarding the mechanisms underlying the micro-bubble carpet and oscillations.
A detailed look was also taken on the dynamics of single hydrogen bubbles in microgravity during parabolic flights. Three bubble evolution scenarios were identified depending on the electric potential applied and the acid concentration. The dominant scenario, characterised by lateral detachment of the grown bubble, was studied in detail. For that purpose, the evolution of the bubble radius, electric current and bubble trajectories as well as the bubble lifetime were comprehensively addressed for different potentials and electrolyte concentrations. The bubble-bubble coalescence events, which are responsible for reversals of the direction of bubble motion, were particularly analysed. Finally, as parabolic flights also permit hypergravity conditions, a detailed comparison of the characteristic bubble phenomena at various levels of gravity was drawn.
Finally, the Marangoni convection at the foot of hydrogen gas bubbles mainly induced by the thermocapillary effect is systematically studied during the bubble evolution, the bubble position oscillations, at horizontal and tilted electrodes both in terrestrial and hyper-g environments. The flow structure progressively modifies with the bubble evolution or during the bubble position oscillations, i.e. as per electric current and bubble geometry variation. The velocity increases both with the bubble size and the electric current magnitude. It reaches up to 50 mm/s and 125 mm/s shortly before the bubble detachment at horizontal and tilted electrodes, correspondingly. The bubble position oscillations characterised by the large variation of the electric current govern the velocity of around ~80 mm/s at the highest and ~40 mm/s at the lowest positions. In the case of tilted electrodes, both in terrestrial and hyper-g environments, the lateral movement of the bubble enables higher values of the current and, therefore, stronger convection. The non-homogeneous distribution of the electric current lines at the tilted electrode results in the asymmetrical Marangoni convection around the bubble. There is a certain limitation in terms of the maximal magnitude of the velocity at different tilt angles, governed by the optimal size of the bubble and electric current. At last, the effects of the particles and laser used for PTV measurements were shown to reduce the duration of the oscillations and to retard the bubble evolution. Both effects were considered during the measurements.
| Identifer | oai:union.ndltd.org:DRESDEN/oai:qucosa:de:qucosa:86932 |
| Date | 28 August 2023 |
| Creators | Bashkatov, Aleksandr |
| Contributors | Eckert, Kerstin, Krug, Dominik, Brinkert, Katharina, Yang, Xuegeng, Dresden University of Technology |
| Source Sets | Hochschulschriftenserver (HSSS) der SLUB Dresden |
| Language | English |
| Detected Language | English |
| Type | info:eu-repo/semantics/publishedVersion, doc-type:doctoralThesis, info:eu-repo/semantics/doctoralThesis, doc-type:Text |
| Rights | info:eu-repo/semantics/openAccess |
| Relation | 10.1103/PhysRevLett.123.214503, 10.1039/D1CP00978H, 10.1103/PhysRevE.106.035105, 10.1039/D2CP02092K, 10.1016/j.electacta.2020.136461, 10.1016/j.ijheatmasstransfer.2023.124466, info:eu-repo/grantAgreement/Federal State of Saxony/European Regional Development Fund/H2-EPF-HZDR//Experimentplattformen für neue Konzepte der Herstellung, Speicherung und energietechnischen Nutzung von Wasserstoff |
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