University of Michigan, Ann Arbor, MI, 48109, USA

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University of Michigan, Ann Arbor, MI, 48109, USA Effects of inter-pulse residual species on discharges in packed bed reactors* Juliusz Kruszelnicki, Kenneth W. Engeling, John E. Foster, and Mark J. Kushner University of Michigan, Ann Arbor, MI, 48109, USA jkrusze@umich.edu, kenengel@umich.edu, jefoster@umich.edu, mjkush@umich.edu MIPSE OCTOBER 2016 * Work supported by the Department of Energy Office of Fusion Energy Science and the National Science Foundation.

University of Michigan Institute for Plasma Science & Engr. AGENDA Introduction to Plasma Packed Bed Reactors for Gas Reprocessing. Descriptions of the model and experiment. Description of Discharge Evolution. Gas Properties: Photoionization Gas Temperature Properties of Packing Material: Secondary Electron Emission Dielectric Constant Concluding Remarks. Application for atm discharges University of Michigan Institute for Plasma Science & Engr. MIPSE_2016

University of Michigan Institute for Plasma Science & Engr. PACKED BED REACTORS Pebbles (or beads) of high dielectric constant provides electric field enhancement. Discharge occurs between and on surfaces of beads. Plasmas in Packed Bed Reactors (PBRs) are used for: Ozone generation CO2 & CO conversion VOC (e.g., benzene, acetaldehyde, p-xylene, toluene) removal Application for atm discharges www.dieselnet.com, www.intechopen.com X. Tu et al., Trans. Plasma Sci. 39, 2172, (2011). University of Michigan Institute for Plasma Science & Engr. NSF_Brief_2016

COLLABORATION: OBJECTIVES Experiment Modeling 2D PBR: visual inspection. Describe breakdown mechanisms. Characterize types of discharges in PBRs. Understand means of reactant production in plasmas in PBRs. Validate models with experiments. Improve operation of PBRs. Application for atm discharges University of Michigan Institute for Plasma Science & Engr. MIPSE_2016

University of Michigan Institute for Plasma Science & Engr. MODEL: nonPDPSIM Plasma Hydrodynamics Poisson’s Equation Gas Phase Plasma Bulk Electron Energy Transport Kinetic “Beam” Electron Transport Unstructured mesh. Fully implicit plasma transport. Time slicing algorithms between plasma and fluid timescales. Neutral Transport Navier-Stokes Neutral and Plasma Chemistry Radiation Transport Surface Chemistry and Charging Ion Monte Carlo Simulation University of Michigan Institute for Plasma Science & Engr. MIPSE_2016 5 5

DESCRIPTION OF EXPERIMENT 2-D Packed Bed Reactor Width: 0.8 cm Length: 1 cm Depth: 0.5 cm Pin-to-planar electrodes. Dielectric rods. K. Engeling et al. Application for atm discharges University of Michigan Institute for Plasma Science & Engr. MIPSE_2016

University of Michigan Institute for Plasma Science & Engr. BASE CASE CONDITIONS Mesh, geometry, and initial electric field. Reaction mechanism: N2/O2/H2O, 35 species, 143 reactions. 12,746 nodes. Photoionization of O2 by radiation from N2** Humidity: University of Michigan Institute for Plasma Science & Engr. MIPSE_2016

BASE CASE – DISCHARGE EVOLUTION Initial negative streamer enters lattice. Regions of field enhancement experience positive restrikes. Standing filamentary microdischarges (FMs) form. Surface charging destabilizes FMs. Surface ionization waves (SIWs) form. Peak electron density near dielectric surfaces. Humidity: University of Michigan Institute for Plasma Science & Engr. MIPSE_2016

BASE CASE – DISCHARGE EVOLUTION Initial negative streamer enters lattice. Three main discharges: Positive restrikes. Filamentary microdischarges (FMs). Surface ionization waves (SIWs). Humidity: Experiment Model University of Michigan Institute for Plasma Science & Engr. MIPSE_2016

BASE CASE – DISCHARGE EVOLUTION Experiment: Optical imaging of discharge formation. 5ns gate. Model: Electron density evolution. 4-decade log scale, 1×1015 cm-3 peak value. Humidity: University of Michigan Institute for Plasma Science & Engr. MIPSE_2016

BASE CASE – REACTIVE SPECIES Inventory (volume integral) of reactive species depends on transient events as discharge propagates through PBR. Positive restrikes and SIWs produces spikes in densities. Differences in species’ dependences based precursor reactions. Humidity: University of Michigan Institute for Plasma Science & Engr. MIPSE_2016

REACTIVE SPECIES: DEPENDENCE ON DISCHARGE TYPE Reactant inventories, electron density. Restrikes (I) produce more N. FMs (II), SIWs (III) produce O. Restrikes include hot electrons O2+e-(5 eV)→O+O+e- N2+e-(12 eV)→N+N+e- Type of discharge affects selectivity. University of Michigan Institute for Plasma Science & Engr. MIPSE_2016

University of Michigan Institute for Plasma Science & Engr. GAS FLOW: VELOCITY Gas velocity distribution for different SCCM flow rates. PBRs use gas flow to collect products in repetitively pulsed discharges. Stagnant regions form where flow is shielded by dielectric. Humidity: University of Michigan Institute for Plasma Science & Engr. MIPSE_2016

GAS FLOW: PRE-IONIZTION Total density of charge species at the end of 1 ms inter-pulse period. Gas flow redistributes reactants from previous pulse which affects both propagation of plasma and production of reactants. Ions, electrons and excited states flow downstream between pulses. With low gas flow, large degree of pre-ionization remains between pulses. Humidity: University of Michigan Institute for Plasma Science & Engr. MIPSE_2016

GAS FLOW: DISCHARGE FORMATION Electron density during third pulse for different SCCM flow rates. Discharge follows plume of pre-ionization and reactants (lower ionization potential) from previous pulse. High gas pressure gradients required to drive high flow rates decrease discharge propagation speed. Pre-charged gas is easier to breakdown leading to increased energy efficiency. Humidity: University of Michigan Institute for Plasma Science & Engr. MIPSE_2016

GAS FLOW: REACTIVE SPECIES Due to differences in mass, different species evacuate at different rates. Each also shot ‘sees’ different species. Both factors impact selectivity. University of Michigan Institute for Plasma Science & Engr. MIPSE_2016

PULSE FREQUENCY: PREIONIZATION Positive ions after inter-pulse periods: 1 ms, 0.1 ms, and 10 μs. The important scaling is (residence time)/(pulse period). Higher frequency (short pulse period) has a similar effective impact as low gas flow (long resident time). Humidity: University of Michigan Institute for Plasma Science & Engr. MIPSE_2016

PULSE FREQUENCY: PREIONIZATION Electron densities at the end of third pulse at different frequencies. Plumes of preionization cause breakdown in different regions – more uniform discharges seen with high frequencies. Humidity: University of Michigan Institute for Plasma Science & Engr. MIPSE_2016

PRF - PRODUCTION OF REACTIVE SPECIES Inventories of reactive species at different frequencies. At high frequency, reactive species do not flow out of plasma zone between pulses. Next pulse "sees" different set of species. Selectivity in producing reactants in part determined by number of pulses each volume element sees. 1 kHz 10 kHz University of Michigan Institute for Plasma Science & Engr. MIPSE_2016

University of Michigan Institute for Plasma Science & Engr. CONCLUDING REMARKS Pre-ionization plays a crucial role in discharge development in PBRs. Reactive species are evacuated by gas flow. At low gas flow rates, densities build up and saturate. High frequency allows for build up of charge, leading to easier breakdown. Each pulse sees different set of species. University of Michigan Institute for Plasma Science & Engr. MIPSE_2016