Atmospheric pressure plasma jets (APPJs) have attracted considerable attention over the last decade, specifically for use in surface engineering. A comparative study of an APPJ, driven by pulsed DC voltage, is conducted in order to examine the plasma impingement onto different surfaces. In this paper, the effect of gas flow rate and composition is investigated using three kinds of substrates: dielectric glass, distilled water and metal plate using fast imaging. Alongside discharges associated with rising and falling voltage, a so-called third discharge is observed during the pulse for water and metal surfaces which corresponds to a restrike breakdown from surfaces to nozzle. The differences in plasma dynamics observed are mainly attributed to the differences in substrate conductivity. In addition, spatial and temporal distributions of OH and O density are investigated by means of laser induced fluorescence (LIF). The OH/O LIF intensity is found to be much higher for metal and water substrates compared to the glass plate. We attribute this effect to the differences in power dissipation associated with the presence and intensity of the third discharge. Effects of gas flow rate and seed gas (H 2 O and O 2 ) mixing on the LIF enhancement are also studied. The related results provide additional insights for optimizing the generation of reactive species.

In this work, the dependence of the length of plasma plume, propagation velocity, electric field in the streamer head, and propagation mode transition on the tube diameter varied in the range of 0.07–4 mm is investigated for the first time. The atmospheric-pressure helium plasma plume, ignited by a positive pulsed direct current voltage with a pulse rising time of 60 ns, is confined inside a long glass tube. First, the decreased tube diameter results in the reduction of the length of plasma plume but the growth of aspect ratio of plasma plume. Second, as the tube diameter decreases, the average velocity of the propagation of plasma plume increases first, then reaches a maximum value at tube diameter of 1 mm, and finally decreases for the tube diameter decreasing further. Third, the electric field in the streamer head, determined by the method based on Stark polarization spectroscopy of He 447 nm line, increases monotonically from 9 kV/cm to 20 kV/cm with the tube diameter decreasing from 4 mm to 0.6 mm. Finally, when the tube diameter is further reduced to 0.07 mm, high-speed photography reveals that the propagation mode of the plasma plume transits from the plasma bullet to the continuous plasma column.

Plasmas interacting with liquids enable the generation of a highly reactive interfacial liquid layer due to a variety of processes driven by plasma-produced electrons, ions, photons, and radicals. These processes show promise to enable selective, efficient, and green chemical transformations and new material synthesis approaches. While many differences are to be expected between conventional electrolysis and plasma–liquid interactions, plasma–liquid interactions can be viewed, to a first approximation, as replacing a metal electrode in an electrolytic cell with a gas phase plasma. For this reason, we refer to this method as plasma-driven solution electrochemistry (PDSE). In this Perspective, we address two fundamental questions that should be answered to enable researchers to make transformational advances in PDSE: How far from equilibrium can plasma-induced solution processes be driven? and What are the fundamental differences between PDSE and other more traditional electrochemical processes? Different aspects of both questions are discussed in five sub-questions for which we review the current state-of-the art and we provide a motivation and research vision.

While plasma-liquid interactions have been an important focus in the plasma research community, the impact of the strong coupling between plasma and liquid on plasma properties and processes remains not fully understood. In this work, we report on the impact of the applied voltage, pulse width and liquid conductivity on the plasma morphology and the OH generation for a positive pulsed DC atmospheric pressure plasma jet with He-0.1% H2O mixture interacting with a liquid cathode. We adopted diagnostic techniques of fast imaging, 2D laser induced fluorescence (LIF) of OH and Thomson scattering spectroscopy. We show that plasma instabilities and enhanced evaporation occur and have a significant impact on the OH generation. At elevated plasma energies, it is found that the plasma contracts due to a thermal instability through Ohmic heating and the contraction coincides with a depletion in the OH density in the core due to electron impact dissociation. For lower plasma energies, the instability is suppressed/delayed by the equivalent series resistor of the liquid electrode. An estimation of the energy flux from the plasma to the liquid shows that the energy flux of the ions released into the liquid by positive ion hydration is dominant, and significantly larger than the energy needed to evaporate sufficient amount of water to account for the measured H2O concentration increase near the plasma-liquid interface.

Plasmas interacting with liquid microdroplets are gaining momentum due to their ability to significantly enhance the reactivity transfer from the gas phase plasma to the liquid. This is, for example, critically important for efficiently decomposing organic pollutants in water. In this contribution, the role of ⋅OH as well as non-⋅OH-driven chemistry initiated by the activation of small water microdroplets in a controlled environment by diffuse RF glow discharge in He with different gas admixtures (Ar, O2 and humidified He) at atmospheric pressure is quantified. The effect of short-lived radicals such as O⋅ and H⋅ atoms, singlet delta oxygen (O2(a 1Δg)), O3 and metastable atoms of He and Ar, besides ⋅OH radicals, on the decomposition of formate dissolved in droplets was analyzed using detailed plasma diagnostics, droplet characterization and ex situ chemical analysis of the treated droplets. The formate decomposition increased with increasing droplet residence time in the plasma, with ∼70% decomposition occurring within ∼15 ms of the plasma treatment time. The formate oxidation in the droplets is shown to be limited by the gas phase ⋅OH flux at lower H2O concentrations with a significant enhancement in the formate decomposition at the lowest water concentration, attributed to e−/ion-induced reactions. However, the oxidation is diffusion limited in the liquid phase at higher gaseous ⋅OH concentrations. The formate decomposition in He/O2 plasma was similar, although with an order of magnitude higher O⋅ radical density than the ⋅OH density in the corresponding He/H2O plasma. Using a one-dimensional reaction–diffusion model, we showed that O2(a 1Δg) and O3 did not play a significant role and the decomposition was due to O⋅, and possibly ⋅OH generated in the vapor containing droplet-plasma boundary layer.

Plasma is used as a flow visualization method to display the gas flow of a plasma jet. Using this method, it is found that a discharge in a plasma jet promotes the transition of the gas flow to turbulence. A discharge at intermediate frequency (∼6 kHz in this paper) has a stronger influence on the gas flow than that at lower or higher frequencies. Also, a higher discharge voltage enhances the transition of the gas flow to turbulence. Analysis reveals that pressure modulation induced both by the periodically directed movement of ionized helium and Ohmic heating on the gas flow plays an important role in inducing the transition of the helium flow regime. In addition, since the modulations induced by the high- and low-frequency discharges are determined by the frequency-selective effect, only intermediate-frequency (∼6 kHz) discharges effectively cause the helium flow transition from the laminar to the turbulent flow. Moreover, a discharge with a higher applied voltage makes a stronger impact on the helium flow because it generates stronger modulations. These conclusions are useful in designing cold plasma jets and plasma torches. Moreover, the relationship between the discharge parameters and the gas flow dynamics is a useful reference on active flow control with plasma actuators.

Cold atmospheric pressure plasma jets (APPJs) enable the generation of a large flux of highly reactive species to heat sensitive substrates at near ambient temperatures. Nonetheless, the experimental determination of reactive species inside APPJs, while exceedingly important, has not been reported in significant detail. In this work, we report the time-resolved axial density of hydroxyl (OH) and hydrogen radicals (H) in an APPJ device and its effluent operating in a He–H2O mixture using 1D laser induced fluorescence (LIF) and two-photon absorption LIF (TALIF). The results show that H and OH are mainly generated between the electrodes in the APPJ rather than by the guided streamer. The produced H and OH inside the jet are convectively transported to the jet effluent and determine the H and OH densities in jet effluent. The dominant production and destruction mechanisms of H and OH were obtained from a 0D model. The different production mechanisms of H and OH can explain the change in memory effect observed for OH (and not for H) for varying pulse repetition rates of the plasma generation.

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