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Nayak, Gaurav

Publications and source records attributed to Nayak, Gaurav.

HCOO - aq Degradation in Droplets by OH aq in an Atmospheric Pressure Glow Discharge

Plasmas in contact with liquids can degrade organic molecules in solution, as reactive oxygen and nitrogen species produced in the plasma solvate into the liquid. Immersing small droplets (tens of microns in diameter) in the plasma can more rapidly activate the liquid compared to treating a large volume of liquid with a smaller surface-to-volume ratio. The interactions between a radio frequency glow discharge sustained in He/H 2 O and a water droplet containing formate (HCOO - aq ) immersed in and flowing through the plasma were modeled using a 0-dimensional global plasma chemistry model to investigate these activation processes. HCOO - aq interacts with OH aq , produced from solvation of OH from the gas phase. HCOO - aq concentrations were benchmarked with previously reported experimental measurements. The diameter of the droplet, initial HCOO - aq concentration, and gas flow rate affect only the HCOO - aq concentration and OH aq density, leaving the OH density in the gas phase unaffected. Power deposition and gas mixture (e.g., percentage of H 2 O) change both the gas and liquid phase chemistry. A general trend was observed – during the first portion of droplet exposure to the plasma, OH aq primarily consumes HCOO - aq . However, O2 - aq , a byproduct of HCOO - aq consumption, consumes OH aq once O2 - aq reaches a critically large density. Using HCOO - aq as a surrogate for OH aq sensitive contaminants, combinations of residence time, droplet diameter, water vapor density, and power will determine the optimum remediation strategy.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Non‐OH‐driven liquid‐phase chemistry in water microdroplets

Abstract Water microdroplets containing organic and fluorinated compounds, such as formate, perfluorooctanoic acid (PFOA) and triflic acid, were exposed to a radiofrequency glow discharge plasma with a droplet residence time on the order of milliseconds. Triflic acid remained unaffected by any plasma condition while >75% decomposition of formate and PFOA could be achieved. In situ hydroxyl (OH)‐laser‐induced fluorescence measurements near the droplets confirmed that the conversion was independent of the OH flux to the droplet. A series of control experiments suggest that the contribution of vacuum UV photons in such decomposition of aqueous compounds can be significant for He and He + 17% Ar plasmas and can also explain unexpected decomposition trends as a function of droplet residence time in the plasma.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Sheath formation around a dielectric droplet in a He atmospheric pressure plasma

Interactions at the interface between atmospheric pressure plasmas and liquids are being investigated to address applications ranging from nanoparticle synthesis to decontamination and fertilizer production. Furthermore, many of these applications involve activation of droplets wherein the droplet is fully immersed in the plasma and synergistically interacts with the plasma. To better understand these interactions, two-dimensional modeling of radio frequency (RF) glow discharges at atmospheric pressure operated in He with an embedded lossy dielectric droplet (tens of microns in size) was performed. The properties of the sheath that forms around the droplet were investigated over the RF cycle. The electric field in the bulk plasma polarizes the dielectric droplet while the electron drift in the external electric field is shadowed by the droplet. The interaction between the bulk and sheath electric fields produces a maximum in E/N (electric field/gas number density) at the equator on one side of the droplet where the bulk and sheath fields are aligned in the same direction and a minimum along the opposite equator. Due to resistive heating, the electron temperature T e is maximum 45° above and below the equator of the droplet where power deposition per electron is the highest. Although the droplet is, on the average, negatively charged, the charge density on the droplet is positive on the poles and negative on the equator, as the electron motion is primarily due to diffusion at the poles but due to drift at the equator.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Self-organized patterns at the plasma–liquid anode interface in a helium glow discharge: temporal development and mechanisms

Self-organization at the plasma–liquid anode interface is a commonly observed phenomenon for atmospheric pressure glow plasmas, resulting in patterns with distinctive shapes such as circular ring, star-shaped, and gear-like structures, depending primarily on the discharge current and solution conductivity. Recent studies have shown that the electrode gap distance, solute used for liquid anode solution, and gas composition can also significantly impact pattern formation. Nonetheless, an overarching model or explanation of the key underlying mechanisms consistent with all experimentally observed trends is not yet reported. We propose a key underlying mechanism enabling pattern formation motivated by a detailed parametric study of pattern formation complemented by the temporal development of patterns and consistent with all observed trends. Pattern formation was observed to be on a time scale of 100 μs, similar to the time scales of gas heating and evaporation. It was found that a minimum water evaporation rate of (3.5 ± 0.5) × 10 –6 kg s –1 and reduced electric field in the positive column of 16.6 ± 0.4 Td is required for pattern formation in the investigated cases irrespective of solution conductivity and gas composition for NaCl solutions. Nonetheless, the presence of cations for which the corresponding metal atom has a low ionization energy was identified as a necessary condition for pattern formation. Furthermore, the reported results suggest that the presence of a small amount of metal atoms in the gas phase with low ionization energy enhances the overall ionization rate in the near anode region which triggers pattern formation.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Plasma-droplet interaction study to assess transport limitations and the role of • OH, O • ,H • ,O 2 (a 1 Δ g ),O 3 , He(2 3 S) and Ar(1s 5 ) in formate decomposition

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, O 2 and humidified He) at atmospheric pressure is quantified. The effect of short-lived radicals such as O• and H• atoms, singlet delta oxygen (O 2 (a 1 Δ g )), O 3 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 H 2 O 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. Here, the formate decomposition in He/O 2 plasma was similar, although with an order of magnitude higher O• radical density than the •OH density in the corresponding He/H 2 O plasma. Using a one-dimensional reaction–diffusion model, we showed that O 2 (a 1 Δ g ) and O 3 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.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Non-Thermal Plasma as a Novel Strategy for Treating or Preventing Viral Infection and Associated Disease

Pathogenic viruses cause many human, animal, and plant diseases that are associated with substantial morbidity, mortality and socio-economic impact. Although effective strategies for combatting virus transmission and associated disease are available, global outbreaks of viral pathogens such as the virus responsible for the COVID-19 pandemic demonstrate that there is still a critical need for new approaches that can be used to interrupt the chain of viral infection and mitigate virus-associated pathogenesis. Recent studies point to non-thermal plasma (NTP), a partly ionized gas comprised of a complex mixture of reactive oxygen and nitrogen species along with physical effectors, as the potential foundation for new antiviral approaches. A more thorough understanding of the antiviral properties and safety of NTP has stimulated explorations of NTP as the basis for treatments of viral diseases. The recently described immunomodulatory properties of NTP are also being evaluated for potential use in immunotherapies of viral diseases as well as in antiviral vaccination strategies. In this review, we present the current state-of-the-art in addition to compelling arguments that NTP merits further exploration for use in the prevention and management of viral infections and associated diseases.

60 APPLIED LIFE SCIENCES↗

Controlled plasma–droplet interactions: a quantitative study of OH transfer in plasma–liquid interaction

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% H 2 O 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. Here, 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.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗