An official website of the United States government
Abstract Enhancing mass transport of reactive species and photons at the plasmaliquid interface is an important consideration for the scaling of atmospheric pressure plasmas studied in the laboratory to real-world applications. It is well-known that the introduction of turbulence at any interface will enhance mixing by enhancing species uptake from the gas phase to the liquid phase by surface renewal processes, entrainment, bubbles and surface area modification. The goal of this work is to isolate surface effects associated with turbulence from the multitude of turbulent transport enhanced processes by artificially introducing surface perturbations using Faraday waves. Experiments were also conducted to determine decoloration rate constants of a model contaminant (methylene blue) as a function of both discharge features and hydrodynamics (Faraday surface wavelengths). The local plasma ionization wave at the interfacial structure was modeled and compared to experiments. Interestingly, it was found in experiments that plasma in contact with the water also generated capillary waves thus modifying the surface as well. Plasma ionization waves in combination to acoustic driven Faraday waves adds to the complexity of interpreting the effects of, for example, surface area increases, due to these complex coupled phenomenon. Local plasma ionization wave structure appears to be modified (increased propagation distance) when the liquid is perturbed, leading to increased contact of the liquid water surface with reactive species. Along with interfacial surface area growth, nonlinear convective transport is also increased with perturbations, leading to the general realization that acoustic perturbations can improve transport and thus decoloration of the model contaminant dye.
more »
« less
This content will become publicly available on January 1, 2026
Recent Insights Into Interfacial Transport and Chemical Reactions of Plasma‐Generated Species in Liquid
ABSTRACT The chemistry of plasma–liquid interactions involves a complex interplay of physical and chemical processes at the plasma–liquid interface. These interactions give rise to the generation, transport, and transformation of various reactive species. Since the publication of the Lorenz Roadmap in 2016, significant progress has been made in understanding the interfacial transport and coupled reactions of plasma‐generated species with inorganic and organic compounds. However, critical aspects of plasma–liquid chemistry and mass transfer still require further investigation. This review summarizes recent work on processes at the plasma–liquid interface and the coupled reactions in the liquid phase. We highlight key findings related to the involvement of O atoms, H radicals, solvated electrons, photons, and nitrogen‐derived species at the interface and within the bulk liquid.
more »
« less
- Award ID(s):
- 2318494
- PAR ID:
- 10630150
- Publisher / Repository:
- Wiley
- Date Published:
- Journal Name:
- Plasma Processes and Polymers
- Volume:
- 22
- Issue:
- 1
- ISSN:
- 1612-8850
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
Nonthermal plasmas in contact with liquids have been shown to generate a variety of reactive species capable of initiating reduction–oxidation (redox) reactions at the electrochemically active plasma–liquid interface. In conventional electrochemical cells, selective redox chemistry is achieved by controlling the reduction potential at the solid electrode–electrolyte interface by applying a bias via an external circuit. In the case of plasma–liquid systems, an analogous means of tuning the reduction potential near the interface has not clearly been identified. When treated as a floating surface, the liquid is expected to adopt a net negative charge to balance the flux of hot electrons and relatively cold positive ions. The reduction potential near the plasma–liquid interface is hypothesized to be proportional to the floating potential, which can be approximated using an analytical model provided the plasma parameters are known. Herein, we present a framework for correlating the electron density and electron temperature of a noble gas plasma jet to the reduction potential near the plasma–liquid interface. The plasma parameters were acquired for an argon atmospheric plasma jet in contact with an aqueous solution by means of laser Thomson scattering. The reduction potential was determined using identical reference electrodes to measure the potential difference between the plasma–liquid interface and bulk solution. Interestingly, the measured reduction potentials near the plasma–liquid interface were found to be in good agreement with the model-predicted values determined using the plasma parameters obtained from the Thomson scattering experiments.more » « less
-
Abstract The interactions between plasma and liquid solutions give rise to the formation of chemically reactive species useful for many applications, but the mass transport in the interfacial region is usually limited and not fully understood. In this work, we report on the observation and explanation of droplet ejection at the plasma–liquid interface of a one-atmosphere glow discharge with the liquid anode. The impact of droplets emission on plasma properties is also analyzed by spectroscopy. The process, which is an efficient mass and charge transport mechanism, apparently occurs during discharge operation and thus constitutes a feedback vehicle between the discharge and the liquid. Distinctive from the well-known Talyor cone droplets associated with liquid cathodes, the observed droplets originate from the bubbles due to electrolysis and solvated air which does not require strong electric field at liquid surface. Instead, the droplets are ejected by bubble cavity rupture at the plasma–liquid interface and their size, initial speed are strongly dependent on the gravity, inertia and capillarity. The droplets emerge near the plasma attachment and are subsequently vaporized, emitting intense UV and visible light, which originated from excited OH radicals and sodium derived from the liquid electrolyte. Spectroscopy analysis confirmed that the bursting droplets generally reduce the gas temperature while their effects on electron density depend on the composition of the liquid anode. Results also show that droplets from NaCl solution increase the plasma electron density due to the lower ionization potential of sodium. These findings reveal a new mechanism for discharge maintenance and mass transport as well as suggest a simple approach to dispersing plasma-activated liquid into the gas phase and thus enhancing plasma–liquid interaction.more » « less
-
Abstract. Snow in the environment acts as a host to rich chemistry and provides a matrix for physical exchange of contaminants within the ecosystem. The goal of this review is to summarise the current state of knowledge of physical processes and chemical reactivity in surface snow with relevance to polar regions. It focuses on a description of impurities in distinct compartments present in surface snow, such as snow crystals, grain boundaries, crystal surfaces, and liquid parts. It emphasises the microscopic description of the ice surface and its link with the environment. Distinct differences between the disordered air–ice interface, often termed quasi-liquid layer, and a liquid phase are highlighted. The reactivity in these different compartments of surface snow is discussed using many experimental studies, simulations, and selected snow models from the molecular to the macro-scale. Although new experimental techniques have extended our knowledge of the surface properties of ice and their impact on some single reactions and processes, others occurring on, at or within snow grains remain unquantified. The presence of liquid or liquid-like compartments either due to the formation of brine or disorder at surfaces of snow crystals below the freezing point may strongly modify reaction rates. Therefore, future experiments should include a detailed characterisation of the surface properties of the ice matrices. A further point that remains largely unresolved is the distribution of impurities between the different domains of the condensed phase inside the snowpack, i.e. in the bulk solid, in liquid at the surface or trapped in confined pockets within or between grains, or at the surface. While surface-sensitive laboratory techniques may in the future help to resolve this point for equilibrium conditions, additional uncertainty for the environmental snowpack may be caused by the highly dynamic nature of the snowpack due to the fast metamorphism occurring under certain environmental conditions. Due to these gaps in knowledge the first snow chemistry models have attempted to reproduce certain processes like the long-term incorporation of volatile compounds in snow and firn or the release of reactive species from the snowpack. Although so far none of the models offers a coupled approach of physical and chemical processes or a detailed representation of the different compartments, they have successfully been used to reproduce some field experiments. A fully coupled snow chemistry and physics model remains to be developed.more » « less
-
Laser ablation plasma chemistry is governed by a complex interplay between hydrodynamic plasma-gas mixing processes, thermodynamics, and rapid high-temperature chemical reactions. In this work, we investigate the gas-phase oxidation chemistry of ns-laser ablation aluminum plasmas in air using optical spectroscopy combined with advanced multi-physics modeling. Experimental measurements demonstrate the formation of AlO in the plasma plume as early as 1 μs while computational results reveal that several Al x O y species are distributed in the periphery of the plume at even earlier times (<20 ns) in the presence of large temperature gradients and strong shockwaves. Interactions with the ablation crater during rapid plume expansion are shown to initiate vortex formation, followed by mixing dynamics that work to pull AlO into the vortices to react with gas-phase Al to form Al 2 O. Oxygen and several aluminum oxides are simultaneously pulled up through the stem of the fireball, encouraging further intermixing between reacting species and enhanced molecular formation. This work concludes that chemical dynamics in laser ablation plasmas is driven by diffusion processes, concentration gradients, and plume hydrodynamics while strong shockwaves generated during laser ablation do not impede chemical reactions.more » « less
