CONTROLLING REACTIVE OXYGEN AND NITROGEN SPECIES (RONS) PRODUCTION BY ATMOSPHERIC PRESSURE PLASMA JETS USING GAS SHIELDS* Seth A. Norberga), Ansgar Schmidt-Blekerb),

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CONTROLLING REACTIVE OXYGEN AND NITROGEN SPECIES (RONS) PRODUCTION BY ATMOSPHERIC PRESSURE PLASMA JETS USING GAS SHIELDS* Seth A. Norberga), Ansgar Schmidt-Blekerb), Jörn Winterb), Stephan Reuterb), Eric Johnsena) and Mark J. Kushnerc) a)Department of Mechanical Engineering University of Michigan, Ann Arbor, MI 48109, USA norbergs@umich.edu, ejohnsen@umich.edu b)ZIK Plasmatis at the INP Greifswald e.V. Greifswald, Germany c)Department of Electrical Engineering and Computer Science mjkush@umich.edu http://uigelz.eecs.umich.edu 2013 Gaseous Electronics Conference Princeton, New Jersey, 29 September – 4 October 2013 *Work supported by DOE Fusion Energy Science and National Science Foundation and the Federal Ministry of Education and Research (grant# 03Z2DN12)

University of Michigan Institute for Plasma Science & Engr. AGENDA Overview of Atmospheric Pressure Plasma Jets (APPJ) Control of RONS production Description of model Collaborating experiments Formation of RONS Comparison to experiments in controlled environment Concluding remarks University of Michigan Institute for Plasma Science & Engr. GEC 2013

ATMOSPHERIC PRESSURE PLASMA JETS (APPJ) Low-temperature non-equilibrium atmospheric pressure plasma jets provide a means to remotely deliver reactive species to surfaces. In the biomedical field, plasma jets are being studied for use in, Sterilization and decontamination Destruction of proteins Bacteria deactivation Wound healing Plasma jets typically consist of a rare gas seeded with O2 or H2O flowing into room air. Plasma produced excited states and ions react with room air diffusing into plasma jet to generate ROS (reactive oxygen species) and RNS (reactive nitrogen species). In this talk, results from computational investigation of the use of a shielding gas on the production of RONS will be presented. University of Michigan Institute for Plasma Science & Engr. GEC 2013

ATMOSPHERIC PRESSURE PLASMA JETS (APPJ) Figures from ZIK plasmatis at the INP Greifswald Current attempts to optimize the production of reactive species are involve the gas mixture in the jet and controlling the environment surrounding the jet. ZIK plasmatis at the INP Greifswald are using a shielding gas (various combinations of O2, N2) to surround the jet to influence the production of reactive species and potentially to isolate plasma produced species from the ambient. Production of reactive species can be better controlled. University of Michigan Institute for Plasma Science & Engr. GEC 2013

MODELING PLATFORM: nonPDPSIM Poisson’s equation: Transport of charged and neutral species: Charged Species:  = Sharffeter-Gummel Neutral Species:  = Diffusion Surface Charge: Electron Temperature (transport and rate coefficients from 2-term spherical harmonic expansion solution of Boltzmann’s Eq.): University of Michigan Institute for Plasma Science & Engr. GEC 2013 5 5

MODELING PLATFORM: nonPDPSIM Radiation transport and photoionization: Poisson’s equation extended into materials. Photoionization process: He2*  He + He + h O2 + h  O2+ + e, N2 + h  N2+ + e The reaction mechanism includes electrons, over 40 neutral and charged species, and more than 400 reactions. University of Michigan Institute for Plasma Science & Engr. GEC 2013 6 6

nonPDPSIM: NEUTRAL FLUID TRANSPORT Fluid averaged values of mass density, mass momentum and thermal energy density obtained using unsteady, compressible algorithms. Individual neutral species diffuse within the single fluid, and react with surfaces Solution: 1. Unstructured mesh discretized using finite volumes. 2. Fully implicit transport algorithms with time slicing between modules. University of Michigan Institute for Plasma Science & Engr. GEC 2013

EXPERIMENT AND MODEL GEOMETRIES Humid Air or controlled environment The experiment is 99.999% He or Helium plus dopant (O2 or N2) at a few slm flow rates. The experiment flows shield gas of O2, N2 or dry air at a slightly higher flow rate. The model is cylindrically symmetric. The model has similar dimensions as the experiment. University of Michigan Institute for Plasma Science & Engr. GEC 2013

University of Michigan Institute for Plasma Science & Engr. FLOW CONDITIONS He or He/O2 = 99.8/0.2 through center, 4 slm. Four shielding gas curtains: O2 N2 Dry Air Humid Air (79.5/20/0.5) Neutral gas flow only for 25 ms prior to application of voltage. One -8 kV pulse; 5/75/20 ns pulse shape, 100 µs run time, ring electrode is dielectric. University of Michigan Institute for Plasma Science & Engr. MIN MAX GEC 2013

DISCHARGE CHARACTERISTICS He/O2 =99.8/0.2, O2 shield into humid air (79.5/20/0.5 N2/O2/H2O) Plasma bullet moves as an ionization wave propagating in channel made by He/O2. Reset of spatial location of Te coincides with pulse fall. Long lived electric field due to slow dissipation of charged species (O2-, O2+). -8 kV pulse, 0-150 ns Ring electrode is dielectric. University of Michigan Institute for Plasma Science & Engr. Animation Slide MIN MAX Log scale GEC 2013

FORMATION OF RONS (HUMID AIR SHIELD) He/O2=99.8/0.2, humid air shield into humid air. OH created in plume by jet and humid air interaction e + H2O  H + OH + e O3 and OH grow through the humid air shield in the post pulse period. Closest match to the unshrouded jet results. One -8 kV , 5/75/20 ns pulse, followed by 100 µs flow. Animation Slide MIN MAX Log scale University of Michigan Institute for Plasma Science & Engr. GEC 2013

FORMATION OF RONS (O2 SHIELD) He/O2=99.8/0.2, O2 shield into humid air. Highest production of ROS species. NO effectively blocked. O2(a) and O are formed from electron impact with O2 at intersection of ionization wave with shield. O3 formed as O atoms contact O2 shield gas. Small OH from diffusion of H2O. One -8 kV , 5/75/20 ns pulse, followed by 100 µs flow. University of Michigan Institute for Plasma Science & Engr. Animation Slide MIN MAX Log scale GEC 2013

FORMATION OF RONS (N2 SHIELD) He/O2=99.8/0.2, N2 shield into humid air. Highest production of NO. NO produced by dissociation of N2 by electron impact and reaction with O2 seed. e + N2  N + N + e N + O2  NO + O Lowest O3 production. One -8 kV , 5/75/20 ns pulse, followed by 100 µs flow. University of Michigan Institute for Plasma Science & Engr. Animation Slide MIN MAX Log scale GEC 2013

FORMATION OF RONS (DRY AIR SHIELD) He/O2=99.8/0.2, dry air shield into humid air. Results reflect the composition of the dry air shield – closer to pure N2, but with O2 influence. O3 grows through the dry air shield in the post pulse period. One -8 kV , 5/75/20 ns pulse, followed by 100 µs flow. University of Michigan Institute for Plasma Science & Engr. Animation Slide MIN MAX Log scale GEC 2013

University of Michigan Institute for Plasma Science & Engr. FORMATION OF RONS All cases had He/O2=99.8/0.2 with shield into humid air. OH is effectively blocked with any “dry” shield gas. NO is blocked effectively by O2. Ozone drops an order of magnitude by the use of the N2 shield. One -8 kV , 5/75/20 ns pulse, followed by 100 µs flow. Species Density (cm-3) Shielding Gas University of Michigan Institute for Plasma Science & Engr. GEC 2013

DESCRIPTION OF EXPERIMENT Helium Experiment exhausts into chamber containing average of injected gases. Ambient gas in model consists of this average mixture University of Michigan Institute for Plasma Science & Engr. MIN MAX GEC 2013

University of Michigan Institute for Plasma Science & Engr. EMISSION 99.8% Helium with 0.2% O2 seed flowing at 4 slm with shield gas of O2. The primary reaction mechanism is: e + O  O(3p3P) + e O(3p3P)  O(3s3S) + hν at 844 nm e + O  O(3p5P) + e O(3p5P)  O(3s5S) + hν at 777 nm University of Michigan Institute for Plasma Science & Engr. Animation Slide MIN MAX Log scale GEC 2013

EMISSION AT 777 NM Pure He Pure He He / O2 He / O2 He / N2 He / N2 N2 Dry Air O2 N2 Dry Air O2 N2 Dry Air O2

EMISSION AT 844 NM Pure He He / O2 He / N2 N2 Dry Air O2 N2 Dry Air O2

PREDICTED VS. ACTUAL BEHAVIOR University of Michigan Institute for Plasma Science & Engr.

University of Michigan Institute for Plasma Science & Engr. CONCLUDING REMARKS Optimizing production of selected reactive species by the use of a shielding gas has promise. NO production can be optimized using a nitrogen shield and oxygen admixture. Ozone and O atom production is best optimized using oxygen shield and admixture. Comparisons with experiment in a controlled environment show agreement of trends and allow for order of magnitude analysis. Future modeling work includes: Flux of reactive species to a surface with and without the shield gas. Interaction between reactive species and a water layer and a cell structure. University of Michigan Institute for Plasma Science & Engr. ICOPS 2013

COMPARISON OF EXPERIMENT AND MODEL Cylindrically symmetric. Helium with and without admixture flows at 4 slm with shielding gas at 5 slm. Flow of gas composition into controlled environment at 5 slm. Flow for 25 ms then plasma ignited and plasma bullet propagates into the flow field. One -8 kV DC pulse with 5/75/20 ns pulse profile. 1 atm Similar dimensions Helium or Helium plus admixture (O2 & N2) at 3 slm. Shield gas is oxygen, nitrogen or dry air at 5 slm. Injected into controlled environment. AC pulse at 850 kHz frequency, 1 atm University of Michigan Institute for Plasma Science & Engr. GEC 2013

University of Michigan Institute for Plasma Science & Engr. EMISSION 99.8% Helium with 0.2% N2 seed flowing at 4 slm Shield gas is O2 (left), dry air (middle) and N2 (right) flowing at 4 slm Similar pulse dynamics O atom emission varies significantly with shroud Animation Slide MIN MAX Log scale University of Michigan Institute for Plasma Science & Engr. GEC 2013

University of Michigan Institute for Plasma Science & Engr. EMISSION 99.999% pure Helium flowing at 4 slm Shield gas is O2 (left), dry air (middle) and N2 (right) flowing at 4 slm Similar pulse dynamics O atom emission varies significantly with shroud Animation Slide MIN MAX Log scale University of Michigan Institute for Plasma Science & Engr. GEC 2013

University of Michigan Institute for Plasma Science & Engr. EMISSION 99.8% Helium with 0.2% O2 seed flowing at 4 slm Shield gas is O2 (left), dry air (middle) and N2 (right) flowing at 4 slm Similar pulse dynamics O atom emission varies significantly with shroud Animation Slide MIN MAX Log scale University of Michigan Institute for Plasma Science & Engr. GEC 2013

PREDICTED VS. ACTUAL BEHAVIOR Delete this slide – see me. University of Michigan Institute for Plasma Science & Engr. GEC 2013

PREDICTED VS. ACTUAL BEHAVIOR University of Michigan Institute for Plasma Science & Engr. GEC 2013

EMISSION AT 777 NM Pure He Pure He He / O2 He / O2 He / N2 He / N2 N2 Dry Air O2 N2 Dry Air O2 N2 Dry Air O2

EMISSION AT 844 NM Pure He He / O2 He / N2 N2 Dry Air O2 N2 Dry Air O2