CARBON DIOXIDE SPLITTING INTO CARBON MONOXIDE AND OXYGEN USING ATMOSPHERIC ELECTRODELESS MICROWAVE PLASMA

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1 Proceedings of the Asian Conference on Thermal Sciences 2017, 1st ACTS March 26-30, 2017, Jeju Island, Korea ACTS-P00295 CARBON DIOXIDE SPLITTING INTO CARBON MONOXIDE AND OXYGEN USING ATMOSPHERIC ELECTRODELESS MICROWAVE PLASMA Hojoong Sun 1, Jungwun Lee 1, Moon Soo Bak 1* 1 Sungkyunkwan University, Seobu-ro 2066, Suwon-si, Kyonggi-do, Republic of Korea Presenting Author: sunhj@skku.edu * Corresponding Author: moonsoo@skku.edu ABSTRACT The usage of carbon dioxide as resources has gained great interest to mitigate the global warming. Previous studies have proposed to exploit the carbon dioxide as chemical storage medium by converting into carbon monoxide and oxygen using electricity either left or from renewable energy sources. In this study, atmospheric electrodeless microwave plasma is produced to decompose the carbon dioxide. Optical emission spectroscopy is carried out to characterize plasma properties, in particular, ro-vibrational temperatures. In addition, a plasma kinetic model has been developed for the detail investigation of plasma splitting of carbon dioxide. KEYWORDS: Atmospheric, Electrodeless, Microwave plasma, Splitting, Carbon dioxide, Carbon monoxide, Optical emission spectroscopy, Temperature diagnostic 1. INTRODUCTION Carbon dioxide is the representative greenhouse gas and regulations on carbon emission become stricter. There are several strategies to mitigate carbon dioxide emission. One category could be the carbon capture and storage and the other is the re-use of carbon dioxide. Recent studies have focused on the re-use of carbon dioxide as a chemical storage. The idea is to decompose the carbon dioxide into a value-added carbon monoxide and oxygen with left electricity using some external sources. A Fridman argued that the dissociation process of carbon dioxide could be highly effective when the step-wise selective excitation of vibrational states is possible.[1] Researchers had tried different types of plasma sources and it seems that microwave plasma has shown the highest energy efficiency in dissociating carbon dioxide.[2] Although the feasibility of atmospheric electrodeless microwave plasma on carbon dioxide splitting has been studied, the characteristics of carbon dioxide microwave plasma has not fully determined. In this study, we carried out optical emission spectroscopy to obtained ro-vibrational temperatures and plasma kinetic simulations to investigate the detail of plasma splitting of carbon dioxide.[3] 2.EXPERIMENT SETUP Figure 1 shows the schematic of experimental setup for the generation of electrodeless microwave plasma in carbon dioxide at atmospheric pressure and plasma emission spectroscopy. A 5kW power supply (alter, SM1250) is connected to a water-cooled magnetron (alter, TM ) that generates 2.45GHz microwave. The generated microwave propagates through an isolator, directional coupler, 3-stub tuner (alter, AG340M3), tapered waveguide (so-called Surfaguide), and movable short circuit (WR340SHORT180A1). The Surfaguide focues the microwave into a small volume to amplify the electro-magnetic field. Once the plasma is produced, nearly all microwave power is coupled to the plasma. 1

2 Fig. 1 Schematic of experimental setup for microwave plasma generation and optical emission spectroscopy The plasma is confined in a quartz tube (plasma reactor) whose inner and outer diameter are 2.7 cm and 3.0 cm, respectively, and the carbon dioxide is injected into the tube with swirling to protect the quartz wall from hot plasma gases. The plasma emission is collected using a lens attached to an optical fiber and dispersed using a 1-meter long monochromator.[4] The spectrum is then recorded by a charge-coupled device camera. During the experiments, the microwave power is fixed at 2 kw and the carbon dioxide flow rates is varied from 5 slpm to 20 slpm. Fig. 2 Photographs of carbon dioxide microwave plasmas at different flow rates 2

3 Fig. 3 Comparison between the measured and simulated emission spectra of C2 swan band at (a) nm (b) nm, (c) nm 3. RESULT Figure 2 shows the photographs of atmospheric electrodeless microwave plasmas produced in carbon dioxide. For fixed microwave power, the length of plasma plume is found to decrease with increased carbon dioxide flow rate. For the ro-vibrational temperature measurements at the plasma region, C2 swan band at three different wavelength regions ( nm, nm, nm) are used. Figure 3 shows the example of measured plasma spectra with fitted spectra. The fitted spectra are obtained using a Boltzmann Equilibrium Spectrum Program (BESP) and Nelder Mead Temperature (NMT) programs developed by University of Tennessee s Space Institute.[5] As seen in Fig. 3, the fitted spectra agree well with the measured. The fitting process is performed for all the tested carbon dioxide flow rates (from 5 slpm and 20 slpm) and the result is presented in Fig. 4 Fig. 4 Ro-vibrational temperatures of carbon dioxide microwave plasma as a function of flow rates 3

4 Fig. 5 Calculated ro-vibrational temperatures and electron temperature from plasma kinetic simulations The temperature at the plasma region is found to be 6000K(±200K) and this temperature is almost independent of the carbon dioxide flow rate. Furthermore, from the results, we found that there exists little difference between the rotational and vibrational temperatures. As the dissociation of carbon dioxide had been expected to be facilitated by vibrational excited state species, this finding indicates that the vibration contribution on carbon dioxide splitting, especially in this type of plasma or plasma condition may be not significant. A relevant plasma kinetic model that considers translational and rotational temperatures of atom/molecules, vibrational temperature of molecule, and electron temperature separately is developed for plasma and post-plasma regions, and the simulations are carried out. The plasma region is modeled as 0-D perfectly-stirred reactor (PSR) and the post-plasma region is modeled as 1-D plug flow reactor (PFR). Figure 5 shows the calculated rotational, vibrational temperatures, and electron temperature from the plasma simulation. Electron temperature and rovibrational temperature are 6000 K and there is little difference between these temperatures, consistent with the measurements. This is because the collisional deactivation of vibrational state species at this high temperature of 6000 K is fast enough to lead to a single temperature value for rotational and vibrational temperatures. Figure 6 shows the species number densities at the plasma region and post-plasma region. At the plasma region, almost all carbon dioxide is found to be dissociated into carbon monoxide and atomic oxygen. However, at the post-plasma region, the dissociated carbon monoxide and atomic oxygen recombine to produce carbon dioxide. Fig. 6 Species number densities of CO2, CO, O, and O2 at the plasma region (left) and the post-plasma region (right) computed using the plasma 0-D PSR and 1-D PFR 4

5 4. CONCLUSIONS Dissociation of carbon dioxide into carbon monoxide and oxygen was studied using plasma emission spectroscopy and plasma kinetic simulations. At the plasma region, the gas temperature was found to be about 6000K(±200K) from the plasma emission spectroscopy and the temperature was independent of carbon dioxide flow rates. From the kinetic simulations, the difference between the rotational and vibrational temperatures of the plasma was found to be negligible as a result of fast relaxation of vibrationally excited species and all carbon dioxide at the plasma region is dissociated into carbon monoxide and atomic oxygen. ACKNOWLEDGMENT This work was supported by National Research Foundation of Korea(NRF) grant funded by the Korea government(msip) (No. 2015R1C1A1A ) REFERENCE [1] A. Fridman, Plasma Chemistry, Cambridge university press. (2008). [2] L.F. Spencer, a D. Gallimore, CO2 dissociation in an atmospheric pressure plasma/catalyst system: a study of efficiency, Plasma Sources Sci. Technol. 22 (2013) doi: / /22/1/ [3] C. Park, J.T. Howe, R.L. Jaffe, G. V. Candler, Review of chemical-kinetic problems of future NASA missions, I: Earth entries, J. Thermophys. Heat Transf. 7 (1994) doi: / [4] T. Silva, N. Britun, T. Godfroid, R. Snyders, A simple spectroscopic method for gas temperature determination in CO2-containing discharges, Opt. Lett. 39 (2014) doi: /ol [5] C.G. Parigger, A.C. Woods, D.M. Surmick, G. Gautam, M.J. Witte, J.O. Hornkohl, Computation of diatomic molecular spectra for selected transitions of aluminum monoxide, cyanide, diatomic carbon, and titanium monoxide, Spectrochim. Acta - Part B At. Spectrosc. 107 (2015) doi: /j.sab

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