Plasmas in contact with liquids are a rich source of OH radicals and have been extensively studied in the last decade to leverage the ability to generate chemically reactive species in gas phase plasmas to decompose organics. Multiphase transfer of OH radicals is highly transport limited and to overcome transport limits, the plasma activation of aerosols, small liquid droplets, interspersed in the plasma has been proposed. In this work, we report a combined experimental and modeling study of a controlled plasma–droplet interaction experiment using a diffuse RF glow discharge in He + 0.2% H2O with detailed plasma diagnostics, ex situ analysis of the plasma-induced chemistry in the droplet containing formate, droplet trajectory and size measurements. This enables a quantitative study of the reactivity transfer of OH from the gas phase plasma to the liquid phase and how its diffusion limitations impact formate decomposition in the water droplet. For a droplet with a diameter of 36 μm, we observed 50% reduction in formate concentration in the droplets after plasma treatment for droplet residence times in the plasma of ∼10 ms. These short droplet residence times in the plasma allow in some cases for droplet size reductions of ∼5% in spite gas temperatures of 360 K. A one-dimensional reaction–diffusion model was used to calculate the OH transport and formate oxidation inside the droplet and was able to predict the conversion of formate by plasma in a droplet without any fitting parameters. The model further shows that formate conversion is dominated by near-interfacial reactions with OH radicals and is limited by diffusion of formate in the droplet. The results show that a controlled plasma–micro-droplet reactor as reported in this study might be an excellent tool for detailed quantitative plasma–liquid interaction studies.

The use of low‐temperature plasmas for bio‐decontamination and sterilization has been gaining increased attention. In this study, a two‐dimensional array of integrated coaxial microhollow micro‐discharges generated in dry air at atmospheric pressure is used to treat metal surfaces (gas‐phase) and solution (liquid‐phase) contaminated with a known concentration of feline calicivirus (FCV). FCV acts as a surrogate for human norovirus, which is responsible for causing outbreaks of acute gastroenteritis in humans. The decontamination efficacy as well as the primary chemical pathways leading to virus inactivation in both the treatments are studied and compared. It is found that the humidity of the bio‐sample for gas‐phase treatment in dry air is required to achieve >5 log10 reduction in FCV titer within 3 min. The gas‐phase FCV inactivation is found to be due to a combination of ozone (O3) and reactive nitrogen species (RNS), most likely NOx. The liquid‐phase FCV inactivation mechanism is pH‐dependent and is primarily due to RNS, most likely acidified nitrites. O3 has a negligible effect on FCV suspended in solution. Previous studies performed in a batch reactor have shown that the inactivation pathways through O3 and RNS are mutually exclusive due to ozone poisoning at high NxOy concentrations. The present study employs a flow‐through system which avoids accumulation of reactive species and allows for the coexistence of NOx and O3 for the gas residence times used in this study, giving rise to these specific inactivation pathways.

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Cold atmospheric pressure plasma has potential as a non-thermal processing technology to decontaminate food and food contact surfaces due to its ability to generate an abundance of reactive oxygen and nitrogen species with antimicrobial attributes at ambient conditions. In this study, we present a comparison on the effectiveness of surface decontamination against feline calicivirus (FCV) and Salmonella spp using four different plasma sources, a dielectric barrier discharge (DBD) in direct contact with the substrate and three remote plasma treatment sources: a 2D DBD, a volumetric DBD and a gliding arc discharge. The plasma sources were all operated in air at atmospheric pressure. The decontamination efficacy was enhanced by the presence of humidity on the sample surface and only direct contact between plasma and samples allowed the inactivation of pathogens on dry substrates. Across all sources, FCV was seen to be more susceptible to the plasma-generated species than Salmonella spp. The diminished effectiveness of the gliding arc discharge compared to the DBDs operating at the same power is most likely due to the low Henry’s law constant of NO, the dominant reactive species generated by the gliding arc. Control experiments illustrate that the co-existence of O3 and NO2, as in the afterglow of the remote DBDs enhances the inactivation compared to the inactivation by O3 or NO2 only. A chemical kinetics model of the plasma effluent and the plasma treatments show a strong correlation between the gas-phase concentration of N2O5 and inactivation of the virus. We experimentally show that the production of N2O5 coincides with the enhanced generation of reactive nitrogen species in the liquid phase.