Plasma-liquid interactions represent a growing interdisciplinary area of research involving plasma science, fluid dynamics, heat and mass transfer, photolysis, multiphase chemistry and aerosol science. This review provides an assessment of the state-of-the-art of this multidisciplinary area and identifies the key research challenges. The developments in diagnostics, modeling and further extensions of cross section and reaction rate databases that are necessary to address these challenges are discussed. The review focusses on nonequilibrium plasmas.

Chemical and bactericidal effects induced by plasma in water upon electro‐spraying through DC‐driven positive transient spark discharge in air were investigated. Inactivation of E. coli was determined in dependence on pH (controlled by buffers) and correlated with chemical changes induced in water. Productions of hydrogen peroxide, nitrites, nitrates, peroxynitrites, and pH changes were determined, and the extent of oxidative stress induced in bacteria was evaluated. The degree of inactivation and oxidative damage of bacteria increased with the increasing acidity of the solution. Acidified nitrites interacting with hydrogen peroxide were determined as the most important bactericidal ROS/RNS agents in plasma‐treated water. A possible role of peroxynitrites, ozone, and metal nanoparticles is discussed.

When cold atmospheric plasma comes into contact with water and biological media, antimicrobial or antitumor effects are induced, representing great potential for applications in biomedicine and agriculture. The need to control and tune the chemical composition and biomedical effects of plasma activated water/media (PAW/PAM) is emerging. By comparing two nonthermal air plasma sources, streamer corona and transient spark, interacting with water in open and closed reactors, and by enhancing the plasma-liquid interaction by water electrospray through these discharges, we demonstrate that the plasma gaseous products strongly depend on the discharge regime, its deposited power and gas flow conditions. The streamer corona strongly leads to the formation of ozone and hydrogen peroxide, while the more energetic transient spark leads to nitrogen oxides and hydrogen peroxide. The gaseous products then determine the chemical properties of the PAW and the dominant aqueous reactive oxygen and nitrogen species (RONS). The production of hydrogen peroxide depends on water evaporation and hydroxyl radical formation, which is determined by the discharge power. A transient spark produces higher concentrations of gaseous and aqueous RONS and induces stronger antibacterial effects than a streamer corona; however, the RONS production rates per joule of deposited energy are comparable for both studied discharge regimes. The net production rate per joule of gaseous nitrogen oxides strongly correlates with that of aqueous nitrites and nitrates. The antibacterial effects of the PAW tested on Escherichia coli bacteria are determined by the aqueous RONS: in the lower power streamer corona, this is ascertained mainly by the dissolved ozone and hydrogen peroxide, and in the higher power transient spark, by the combination of hydrogen peroxide, nitrite and acidic pH, while in the transient spark in the closed reactor it is determined by the acidified nitrites present.

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Reactive oxygen and nitrogen species (RONS) are among the key factors in plasma medicine. They are generated by atmospheric plasmas in biological fluids, living tissues and in a variety of liquids. This ability of plasmas to create a delicate mix of RONS in liquids has been used to design remote or indirect treatments for oncological therapy by treating biological fluids by plasmas and putting them in contact with the tumour. Documented effects include selective cancer cell toxicity, even though the exact mechanisms involved are still under investigation. However, the "right" dose for suitable therapeutical activity is crucial and still under debate. The wide variety of plasma sources hampers comparisons. This review focuses on atmospheric pressure plasma jets as the most studied plasma devices in plasma medicine and compiles the conditions employed to generate RONS in relevant liquids and the concentration ranges obtained. The concentrations of H 2 O 2 , NO 2-, NO 3 and short-lived oxygen species are compared critically to provide a useful overview for the reader.

The selective in vitro anti-tumor mechanisms of cold atmospheric plasma (CAP) and plasma-activated media (PAM) follow a sequential multi-step process. The first step involves the formation of primary singlet oxygen (1O2) through the complex interaction between NO2− and H2O2.1O2 then inactivates some membrane-associated catalase molecules on at least a few tumor cells. With some molecules of their protective catalase inactivated, these tumor cells allow locally surviving cell-derived, extracellular H2O2 and ONOO─ to form secondary 1O2. These species continue to inactivate catalase on the originally triggered cells and on adjacent cells. At the site of inactivated catalase, cell-generated H2O2 enters the cell via aquaporins, depletes glutathione and thus abrogates the cell’s protection towards lipid peroxidation. Optimal inactivation of catalase then allows efficient apoptosis induction through the HOCl signaling pathway that is finalized by lipid peroxidation. An identical CAP exposure did not result in apoptosis for nonmalignant cells. A key conclusion from these experiments is that tumor cell-generated RONS play the major role in inactivating protective catalase, depleting glutathione and establishing apoptosis-inducing RONS signaling. CAP or PAM exposure only trigger this response by initially inactivating a small percentage of protective membrane associated catalase molecules on tumor cells.

We present a study of the streamer-to-spark transition in a self-pulsing dc-driven discharge called a transient spark (TS). The TS is a streamer-to-spark transition discharge with short spark duration (∼10-100 ns), based on charging and discharging of the internal capacity of the electric circuit with repetition frequency 1-10 kHz. The TS can be maintained under relatively low energy conditions (0.1-1 mJ pulse −1). It generates a very reactive non-equilibrium air plasma applicable for flue gas cleaning or bio-decontamination. Thanks to the short spark current pulse duration, the steady-state gas temperature, measured at the beginning of the streamers initiating the TS, increases from an initial value of ∼300 K only up to ∼550 K at 10 kHz. The streamer-to-spark transition is governed by the subsequent increase in the gas temperature in the plasma channel up to ∼1000 K. This breakdown temperature does not change with increasing repetition frequency f. The heating after the streamer accelerates with increasing f , leading to a decrease in the average streamer-to-spark transition time from a few µs to less than 100 ns.

The paper presents an analysis of electrical characteristics of streamer-to-spark transition discharge in air at atmospheric pressure named transient spark (TS). The TS is applicable for flue gas cleaning or bio-decontamination and has potential in plasma shielding, combustion and flow control applications. Despite the dc applied voltage, TS has a pulsed character with short (∼10-100 ns) high current (>1 A) pulses, with repetitive frequencies 1-20 kHz. Estimation of the temporal evolution of electron density shows that n e ≈ 10 16 cm −3 at maximum and ∼10 11 cm −3 on average are reached using relatively low power delivered to the plasma (0.2-3 W). Thanks to the high repetition frequency, n e between two current pulses does not fall below a critical value and therefore plasma exists during the whole time. A detailed analysis of the TS control by electrical circuit parameters is presented. With appropriate circuit components, the current pulse tail (>1 mA) can be extended and the electron density can be held above ∼10 13 cm −3 for several tens of µs.