22nd International Symposium on Plasma Chemistry July 5-10, 2015; Antwerp, Belgium Design and preliminary characterization of an atmospheric pressure glow discharge stamp F.P. Sainct1, N.Y. Mendoza-Gonzalez1, N. Hordy1 and S. Coulombe1 1 Plasma Processing Laboratory - PPL, Department of Chemical Engineering, McGill University, Montréal, Québec, Canada Abstract: The design of a 1.5 cm2 low-power atmospheric pressure glow discharge stamp (APDG-s) and the results of its preliminary fluid dynamic and spectroscopic characterization are presented. Operation of the APGD-s was stable and produced an uniform flowing afterglow over a range of continuous RF (13.56 MHz) powers (10-20 W) and He flow rates (6-24 L/min). Computational fluid dynamics and optical emission spectroscopy analyses showed that the He flow entrains and mixes surrounding air, resulting in the large production of radicals. Keywords: non-thermal plasma, flowing atmospheric pressure afterglow, computational fluid dynamics, optical emission spectroscopy 1. Introduction Nonthermal atmospheric pressure plasma sources are of increasing interest for a wide range of technological applications including plasma medicine, nanoparticle synthesis, plasma chemical functionalization and material deposition [1-3]. A number of configurations have been adopted for sustaining a plasma at atmospheric pressure, and miniature jets are amongst the most popular due to their applicability to a number of treatments [4]. These plasma jets feature a localized zone of treatment often not exceeding a few mm2, and significant gas velocities. In biomedical and surface modification applications, in particular, the treatment of larger surfaces with low-gas flows is often desirable. In an attempt to fill this gap, we designed, built and tested a novel source that produces a low-power flowing afterglow compatible with such application constraints. We used computational fluid dynamics (CFD) simulations and optical emission spectrometry (OES) to assist the design and to perform a preliminary characterization of the Atmospheric Pressure Glow Discharge stamp (APGD-s) operating with He as the main plasma gas. CFD is used to reveal the main flow patterns under cold conditions (no plasma) while spatiallyresolved relative OES is used to reveal the spatial structure of the air entrainment downstream to the source’s exit, as well as the distribution of the excitation temperature in the discharge. 2. Design and characterization methods A picture of the APGD-s is shown in Fig. 1, where it is positioned above a sample for plasma functionalization. The device consists of a plane-to-plane geometry featuring a RF-powered grid-electrode located inside a grounded aluminum support structure, and facing a grounded grid-electrode (grid bar diameter and spacing are 0.3 mm and 0.5 mm, respectively). The main plasma P-II-5-18 gas is injected above in a narrower channel (see Fig. 2). This configuration showed to be efficient at producing radicals and metastable species in the plasma-forming region and transporting the species downstream. The electrode spacing, a critical parameter in this design as it directly impacts the applied electric field, was set to 0.8 mm. We found that an applied continuous wave RF (13.56 MHz) power ranging from 10 to 20 W and total gas flow rates ranging from 6 to 24 L/min provide stable and suitable operating conditions for the intended applications. To ensure compatibility with temperaturesensitive applications, the temperature of the gas at the outlet was measured with a 1 mm RF-shielded thermocouple. Fig. 1. Downstream end of the APGD-s positioned for surface functionalization (helium, outside diameter of the outlet is 14 mm). In order to support the design of the source and to help understand the OES characterization results, the fluid flow in the APGD-s was analysed with the commercial CFD code ANSYS Fluent v14.5 [5]. Because of the cylindrical symmetry of the APGD-s (Fig. 2), a 1 two-dimensional r-z computational geometry was used. The simulations were done with a glass plate facing the exit of the APGD-s in order to mimic plasma functionalization conditions (plate-to-APGD-s distance of 10 mm). An extended area (10 mm in z, and 30 mm in r) was included for the analysis of the effect of surrounded air. The plasma formation and effect of the grid electrodes on the flow pattern were neglected in this preliminary study. From the CFD modelling results, streamlines, which indicate the direction of the fluid flow and existence of recirculation zones, are presented to analyse the flow pattern. Fig. 2 shows the streamlines at 20 L/min (He). Fig. 3. Schematics of the APGD-s and OES setup. Fig. 2. Model geometry of the APDG-s and resulting He streamlines. He flow is set at 20 L/min. The APDG-s is placed 10 mm away from the glass, and the simulation domain radius is 30 mm wide. The combined Navier-Stokes and non-reactive species transport equations were solved in the 2D computational domain composed of 80 000 control volumes. As turbulence can be present due to the two geometry expansions adopted for this design, a standard k-epsilon model was used. The density of the helium-air mixture was calculated with the incompressible ideal gas equation. The boundary conditions are the imposed mass flow rate of helium at the inlet, the non-slip conditions at the wall, and atmospheric static pressure at the outlet. A constant temperature of 300 K was used for the material properties. OES measurements were performed using a 25 cm focal length spectrometer (Acton SpectraPro 2750) equipped with a PiMax camera (Princeton Instruments PIMAX 1024x256). The 1200 grooves/mm grating, blazed at 300 nm, provided a spectral resolution of 0.22 nm. The light emitted by the discharge was collected with a system of two lenses with focal lengths of 50 mm and 100 mm, respectively, as presented on Fig. 3. With this optical setup, the magnification is 0.5. A 200 µm diameter optical fiber, located at the focal point of the imaging lens, was connected to the entrance slit of the spectrometer providing a spatial resolution of 400 µm in the radial direction. 3. Results 2 A first recirculation zone is observed as the gas enters the powered electrode zone because of the geometry expansion. A second recirculation zone is observed in the open area between the APGD-s and glass substrate. This recirculation pattern is responsible for the entrainment of surrounding air into the inter-electrode zone. Fig. 4 shows the radial distribution of the air mass fraction at the grounded electrode location. Obviously, a larger amount of air is observed near the edges but a significant amount finds its way to the centerline (~30%). However it is important to note that the magnitude of the air mass fraction is likely to change with the addition of the wire grid electrodes to the model, as the presence of the two electrode grids breaks up the main gas flow into smaller cells, which may promote mixing with the entrained air. From experimental testing of the APGD-s with a combined He/O 2 flow we can estimate the maximum mass fraction of oxygen to be less than 0.5 %, since the injection of 0.5 % of O 2 with helium significantly changes the plasma behaviour. Fig. 4. Simulated mass fraction of air at the grounded electrode location (z = 13.6 mm). The symmetry of the profile is a consequence of the cylindrical symmetry chosen for the simulation. The full profile is provided to simplify the comparison with Fig. 2. The OES emission spectrum presented in Fig. 5, acquired 4 mm from the center of the discharge, clearly shows that surrounding air is entrained and mixes with the main He P-II-5-18 stream to produce emission bands from OH, N 2 , N 2 + and emission lines from atomic O and He. Fig. 5. Emission spectrum of the He plasma, 4 mm from the center, integrated over 100 ms and 100 accumulations. Results presented in Fig. 6 reveal a rapid decrease of the gas temperature (measured with the thermocouple) with increasing gas flow and decreasing RF power. The observed gas temperature range is compatible with most heat-sensible applications. Fig. 6. Gas temperature evolution with He flow rate and applied RF power. The gas temperature obtained with the thermocouple was compared to the plasma temperature estimated by OES, using the OH, N 2 and N 2 + rotational band emissions over the 300-400 nm range. The Specair software [6, 7] was used to model the experimental OES results and to determine the corresponding rotational and vibrational temperatures. The OH emission spectrum presented in Fig. 6 was well reproduced by the simulation using a rotational temperature relatively close to the gas temperature (400 K), and a high vibrational temperature (5000 K). This high non-equilibrium temperature situation could result from the collision with high-energy P-II-5-18 helium metastables [8]. The same situation is observed with the N 2 (C) and N 2 + emission bands presented in Fig. 8, with a low rotational temperature and a high vibrational temperature. Fig. 7. OH molecular emission spectrum in the center of the discharge at 20 L/min He and 20 W, along with the best fit obtained with Specair. The radial distribution of the optical emission of each species has been studied from the centerline of the APGD-s to its side. The results presented in Fig. 9 show a nearly constant emission intensity for helium across the discharge, whereas the optical emission from air-related species features a strong gradient, with a weaker intensity in the center and stronger emission on the sides. The optical emission from the air-related species increases in the same proportion for all species compared to He emission, which observation suggests a greater air fraction on the side of the APGD-s than in the center. These results are in qualitative agreement with the simulated mass fraction of air shown in Fig. 4. 3 The APGD-s source has been analyzed using CFD and OES diagnostics. CFD was used to better understand the basic flow pattern in the outlet area as well as the mixing of the plasma-forming gas with surrounding air. The simulations showed that a recirculation pattern forms due to the sudden expansion of the geometry and presence of a substrate. This recirculation introduces a small amount of surrounding air in the inter-electrode zone, thus leading to the production of radicals from air. These results are in qualitative agreement with the OES results, which revealed air-related species emission in the plasmaforming zone. A more detailed model considering the plasma-forming zone and a realistic representation of the grid electrodes will be developed to optimize the APGD-s design for specific applications. Fig. 8. Emission spectrum in the center of the discharge at 20 L/min He and 20 W, with the Specair fit of N 2 and N 2 + emission. Fig. 9. Radial distribution of the emission intensity of selected at 20 L/min and 20 W. 4. Conclusion 4 5. Acknowledgements The authors wish to thank C. Szalacsi for his technical assistance. The project was funded by the National Sciences and Engineering Research Council of Canada (NSERC), the Fonds de recherche du Québec – Nature et technologies (FRQNT) and McGill University. 6. References [1] M. Laroussi and A. Tamer. Plasma Process. Polymers, 4, 777-788 (2007) [2] S. Lee, J.-W. Peng and C.-H. Liu. Carbon, 46, 2124-2132 (2008) [3] R.J. Zaldivar, J.P. Nokes, P.M. Adams, K. Hammoud and H.I. Kim. Carbon, 50, 2966-2975 (2012) [4] J.S. Sousa, et al. J. Appl. Phys., 109, 1-8 (2011) [5] ANSYS FLUENT 14.5, Theory Guide. (Ansys, Inc.) [6] C.O. Laux, T.G. Spence, C.H. Kruger and R.N. Zare. Plasma Sources Sci. Technol., 12, 125-138 (2003) [7] www.specair-radiation.net [8] J. Lefebvre and A. Ricard. Rev. Physique Appliquée, 10, 137-142 (1975) P-II-5-18
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