Nanosecond plasmas in liquids play an important role in the field of decontamination, electrolysis or plasma medicine. The understanding of these very dynamic plasmas requires information about the temporal variation of species densities and temperatures. This is analyzed by monitoring nanosecond pulsed plasmas that are generated by high voltages (HVs) between 14 and 26 kV and pulse lengths of 10 ns applied to a tungsten tip with 50 μm diameter immersed in water. Ignition of the plasma causes the formation of a cavitation bubble that is monitored by shadowgraphy to measure the dynamic of the created bubble and the sound speed of the emitted acoustic waves surrounding this tungsten tip. The temporal evolution of the bubble size is compared with cavitation theory yielding good agreement for an initial bubble radius of 25 μm with an initial pressure of 5 × 108 Pa at a temperature of 1200 K for a HV of 20 kV. This yields an initial energy in the range of a few 10−5 J that varies with the applied HV. The dissipated energy by the plasma drives the adiabatic expansion of water vapor inside the bubble from its initial supercritical state to a low pressure, low temperature state at maximum bubble expansion reaching values of 103 Pa and 50 K, respectively. These predictions from cavitation theory are corroborated by optical emission spectroscopy. After igniting the nanosecond plasma, the electrical power oscillates in the feed line between HV pulser and plasma chamber with a ring down time of the order of 60 ns. These reflected pulses re-ignite a plasma inside the expanding bubble periodically. Broadband emission due to recombination and Bremsstrahlung becomes visible within the first 30 ns. At later times, line emission dominates. Stark broadening of the spectral lines of H α (656 nm) and OI (777 nm) is evaluated to determine both the electron density and the electron temperature in these re-ignited plasmas.
Nanosecond plasmas in liquids are an important method to trigger the water chemistry for electrolysis or for biomedical applications in plasma medicine. The understanding of these chemical processes relies on knowing the variation of the temperatures in these dynamic plasmas. This is analyzed by monitoring nanosecond pulsed plasmas that are generated by high voltages at 20 kV and pulse lengths of 15 ns applied to a tungsten tip with 50 μm diameter immersed in water. Plasma emission is analyzed by optical emission spectroscopy ranging from UV wavelengths of 250 nm to visible wavelengths of 850 nm at a high temporal resolution of 2 ns. The spectra are dominated by the black body continuum from the hot tungsten surface and line emissions from the hydrogen Balmer series. Typical temperatures from 6000 K up to 8000 K are reached for the tungsten surface corresponding to the boiling temperature of tungsten at varying tungsten vapor pressures. The analysis of the ignition process and the concurrent spectral features indicate that the plasma is initiated by field ionization of water molecules at the electrode surface. At the end of the pulse, field emission of electrons can occur. During the plasma pulse, it is postulated that the plasma contracts locally at the electrode surface forming a hot spot. This causes a characteristic contribution to the continuum emission at small wavelengths.
Discharges in liquids are the basis of a range of applications in electrochemistry, wastewater treatment, or plasma medicine. One advantage of discharges in water is their ability to produce radicals and molecules directly inside liquid with a high conversion efficiency. In this study, H 2 O 2 production in a 10 ns pulsed discharge in water is investigated. The dynamic of these discharges is based on plasma ignition directly inside liquid followed by the formation of a bubble that expands in time before it eventually collapses. This sequence can be well described by cavitation theory. H 2 O 2 is produced using different plasma conditions varying the treatment time, the pulse frequency between 1 and 100 Hz, and the applied voltage in a range from 15-30 kV. The resulting H 2 O 2 concentration is measured using absorption spectroscopy ex situ based on a colorimetry method. The results indicate that the main parameter controlling the H 2 O 2 production constitutes the applied voltage. The measured concentrations are compared with a global chemistry model simulating the chemistry involved during a single pulse using pressures and temperatures from the cavitation model. In addition, a global chemical equilibrium model for H 2 O 2 creation is evaluated as well. The models show a good agreement with the data.The energy efficiency for the production of H 2 O 2 reaches values up to 2 g/kWh. K E Y W O R D S cavitation theory, discharge in water, global chemistry model, H 2 O 2 production, nanosecond pulsed discharge ---
Nanosecond plasmas in liquids can initiate chemical processes that are exploited in the fields of water treatment, electrolysis or biomedical applications. The understanding of these chemical processes relies on unraveling the dynamics of the variation of pressures, temperatures and species densities during the different stages of plasma ignition and plasma propagation as well as the conversion of the liquid into the plasma state and the gas phase. This is analyzed by monitoring the emission of nanosecond pulsed plasmas that are generated by high voltages of 20 kV and pulse lengths of 10 ns applied to a tungsten tip with 50 μm diameter immersed in water. The spectra are acquired with a temporal resolution of 2 ns and the emission pattern is modelled by a combination of black body radiation from the hot tungsten tip and the pronounced emission lines of the hydrogen Balmer series. The data indicate two contributions of the hydrogen line radiation that differ with respect to the degree of self-absorption. It is postulated that one contribution originates from a recombination region showing strong self absorption and one contribution from an ionization region showing very little self-absorption. The emission lines from the ionization region are evaluated assuming Stark broadening, that yielded electron densities up to 5 × 1025 m−3. The electron density evolution follows the same trend as the temporal evolution of the voltage applied to the tungsten tip. The propagation mechanism of the plasma is similar to that of a positive streamer in the gas phase, although in the liquid phase field effects such as electron transport by tunneling should play an important role.
Nanosecond plasmas in liquids are being used for water treatment, electrolysis, or biomedical applications. The exact nature of these very dynamic plasmas and, most importantly, their ignition physics are strongly debated. The ignition itself may be explained by two competing hypotheses: ignition in water may occur (i) via field effects at the tip of the electrode followed by tunneling of electrons in between water molecules causing field ionization or (ii) via gaseous processes of electron multiplication in nanovoids that are created from liquid ruptures due to the strong electric field gradients. Both hypotheses are supported by theory, but experimental data are very sparse due to the difficulty in monitoring the very fast processes in space and time. In this paper, we analyze nanosecond plasmas in water that are created by applying a positive and a negative polarity to a sharp tungsten electrode. The main diagnostics are fast camera measurements and fast emission spectroscopy. It is shown that plasma ignition is dominated by field effects at the electrode–liquid interface either as field ionization for positive polarity or as field emission for negative polarity. This leads to a hot tungsten surface at a temperature of 7000 K for positive polarity, whereas the surface temperature is much lower for negative polarity. At ignition, the electron density reaches 4×1025 m−3 for the positive and 2×1025 m−3 for the negative polarity. At the same time, the emission of the Hα light for the positive polarity is four times higher than that for the negative polarity. During plasma propagation, the electron densities are almost identical of the order of 1–2×1025 m−3 followed by a decay after the end of the pulse over 15 ns. It is concluded that plasma propagation is governed by field effects in a low density region that is created either by nanovoids or by density fluctuations in supercritical water surrounding the electrode that is created by the pressure and temperature at the moment of plasma ignition.
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