Flow Reactor Studies of Non-equilibrium Plasma Assisted Combustion Kinetics

Flow Reactor Studies of Non-equilibrium Plasma Assisted Combustion Kinetics

Author: Nicholas Tsolas

Publisher:

Published: 2015

Total Pages:

ISBN-13:

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A new experimental facility was developed to study the reactive chemical kinetics associated with plasma-assisted combustion (PAC). Experiments were performed in a nearly isothermal plasma flow reactor (PFR), using reactant mixtures highly diluted in an inert gas (e.g., Ar, He, or N2) to minimize temperature changes from chemical reactions. At the end of the isothermal reaction zone, the gas temperature was rapidly lowered to terminate any continuation in reaction. Product composition as a result of any observed reaction was then determined using ex situ techniques, including non-dispersive infrared (NDIR), and by sample extraction and storage into a multi-position valve for subsequent analysis by gas chromatography (GC). Hydroxyl radical concentrations were measured in situ, using the laser induced fluorescence (LIF) technique. Reactivity maps for a given fuel system were achieved by fixing the flow rate or residence time of the reactant mixture through the PFR and varying the isothermal temperature. Fuels studied were hydrogen, ethylene and C1 to C7 alkane hydrocarbons, to examine pyrolysis and oxidation kinetics with and without the effects of a high-voltage nanosecond pulse duration plasma discharge, at atmospheric pressure from 420 K to 1250 K. In select instances, experimental studies were complimented with detailed chemical kinetic modeling analysis to determine the dominant and rate-controlling mechanisms, while elucidating the influence of the plasma chemistry on the thermal (neutral) chemistry.In the hydrogen oxidation system, no thermal reaction was observed until 860 K, consistent with the second explosion limit at atmospheric pressure, at which point all the hydrogen was rapidly consumed within the residence time of the reactor. With the plasma discharge, oxidation occurred at all temperatures examined, exhibiting a steady increase in the rate of oxidation starting from 470 K, and eventually consuming all the initial hydrogen by 840 K. For ethylene, kinetic results with the discharge indicated that pyrolysis type reactions were nearly as important as oxidative reactions in consuming ethylene below 750 K. Above 750 K, the thermal reactions coupled to the plasma reactions to further enhance the high temperature fuel consuming chemistry. Modeling analysis of plasma-assisted pyrolysis revealed that ethylene dissociation by collisional quenching with electronically-excited argon atoms formed in the presence of the plasma, resulted in the direct formation of acetylene and larger hydrocarbons by way of the ethyl radical. Similarly, during plasma-assisted oxidation, excited argon was able to directly dissociate the initial oxidizer to further enhance fuel consumption, but also facilitate low temperature oxidative chemistry due to the effective production of oxygenated species controlled by R+O2 chemistry. At the highest temperatures, the radical production by neutral thermal reactions became competitive and the effectiveness associated with the plasma coupled chemistry decreased. Under the effects of the plasma, alkane fuels exhibited extended limits of oxidation over the entire temperature range considered, compared to that of the thermal reactions alone. At atmospheric pressure, propane and butane exhibited cool flame chemistry between 420 K to 700 K, which normally occurs at higher pressures (P > 1 atm) for thermally constrained systems. This chemistry is characterized by the alkylperoxy radical formation, isomerization to the hydroperoxyalkyl radical, followed by dissociation to form aldehydes and ketones. Whereas, intermediate temperature chemistry between 700 K to 950 K, is characterized by beta-scission of the initial alkyl radical to form alkenes and smaller alkanes. The culmination of these studies demonstrate new insight into the kinetics governing PAC and provides a new experimental database to facilitate the development and validation of PAC-specific kinetic mechanisms.


Multi-physics Modeling of Electromagnetically Driven Surface Plasma Discharges

Multi-physics Modeling of Electromagnetically Driven Surface Plasma Discharges

Author: Yunho Kim

Publisher:

Published: 2019

Total Pages: 420

ISBN-13:

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This dissertation presents the computational modeling of non-equilibrium plasma discharges on an electromagnetically driven surface and its application to plasma assisted combustion. We address challenges often encountered in high pressure plasma discharges such as the non-uniform formation of plasmas due to filamentations and show how they could be handled by using a particular type of metamaterial. A metamaterial in the present context is an artificial composite assembled with periodic elements smaller than an incident wavelength. Metamaterials have drawn significant interest in engineering communities during the past few decades due to their extraordinary electromagnetic (EM) characteristics, e.g., a negative refractive index, that cannot be naturally excited using conventional methods or materials. An interesting electrodynamic phenomenon associated with metamaterials is the possible surface wave excitation on the artificially engineered surfaces. In particular, by carefully designing the assembly of periodic elements consisting of conductors and dielectrics, a strongly localized surface wave mode known as a spoof surface plasmon polariton (SSPP) can be efficiently excited. The extraordinary electromagnetic property of SSPP is its ability to imitate the behaviors of a surface plasmon polariton (SPP) in a wide range of frequencies (GHz -THz) while SPP can exist only in the optical regime (100's THz). In this study, our goal is to provide the in-depth analysis of the electrodynamics of SSPP, transients of surface plasma generation due to SSPP resonances, and to demonstrate the feasibility of using it for plasma assisted combustion. We have used multiple computational models that have been developed by our group and added necessary features to simulate the phenomena more accurately. In the first part of this work, we describe the numerical schemes employed for simulations. The computational tool consists of solvers for three different sets of equations: Maxwell's equations for high frequency (HF) electromagnetics, plasma governing equations for discharge physics, and reactive Navier Stokes equations for combustion. Coupling of these equations must be done carefully due to the multi-scale nature of the high frequency plasma discharges and combustion. The length and time scales range from micrometers to centimeters and nanoseconds to milliseconds, respectively. We provide the details of the coupling of the equations as well as the discretization methods for each set of equations. In this work, one of chief contributions to improving the models is the implementation of an enhanced version of absorbing boundary condition (CFS-PML) for second order Maxwell's equations. CFS-PML is especially suited for electromagnetic wave simulations that involve conductors which we demonstrate by solving a model problem for the verification of the code. In the second part, we present the computational study of argon surface plasma discharges generated by SSPP. The EM surface wave excitation is first analyzed in depth because the electromagnetic power absorption by electrons determines the transients of plasma breakdown. Electrodynamics of the SSPP excitation is investigated using broadband and monochromatic wave simulations. Instead of the infinite array of periodic elements, we have studied the metamaterial with a finite length for practical engineering applications. It is found that over a wide range of length scales from millimeters to centimeters, the EM waves always have a single node structure at resonance frequencies. The surface wave excited on the metasurface is characteristic of coupling between the cavity mode and surface wave mode. We refer to the resonance pertinent to such coupling as hybrid resonance. The shift of the hybrid resonance frequency is investigated in terms of varying dielectric permittivities, distances between perforations, and the whole lengths of the metasurfaces. Using an optimal configuration of the metasurface, the transients of the surface plasma generation due to the field intensification is studied. Interactions among the surface plasma, SSPP and the incident wave are presented. Multiple simulations show that even if the metasurfaces have different lengths, the transients of surface plasma formation are qualitatively identical at the hybrid resonance frequencies. Such scalability is one of the primary features of metamaterials that can be extended to the plasma discharge. In the third part, plasma assisted combustion induced by microwave sources is studied. Previous research in combustion engineering communities have addressed the importance of volumetric formation of flame kernel for successful combustion. Another key point in plasma assisted combustion is the volumetric generation of radical species in nanosecond timescale, which can significantly reduce the ignition delay for lean fuel-air mixtures. Motivated by the need for mechanisms that can generate combustion enhancing radicals over a large area, we have investigated the feasibility of using the SSPP generated surface plasmas for plasma assisted combustion. A kinetic mechanism of H2 - air mixture that was previously established by our group is used for this study. A mixture with the equivalence ratio of 0.3 at the initial pressure and temperature of 1 atm and 1000 K is assumed, respectively. Fully coupled simulations show that the cm-scale plasma kernel can be efficiently transitioned into successful ignition and flame propagation with shortened ignition delay. In the last part, we discuss strategies to parallelize the simulation tools for high performance computing. The governing equations solved in this study are spatially discretized using either finite edge element method or cell-centered finite volume method. They require different approaches to achieve parallel scalability, and in particular, the Maxwell's equations needs a special preconditioning technique to reduce computational time. The technique is known as nodal auxiliary space preconditioning whose theoretical background and performance on a supercomputer are presented. Additionally, the module which solves reactive Navier-Stokes equations is also parallelized to study large scale (centimeters) ignition phenomena. For both plasma-wave coupled solver and combustion solver, we discuss the details of MPI(Message Passing Interface)-based parallelization processes


Database Needs for Modeling and Simulation of Plasma Processing

Database Needs for Modeling and Simulation of Plasma Processing

Author: National Research Council

Publisher: National Academies Press

Published: 1996-10-21

Total Pages: 74

ISBN-13: 0309175135

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In spite of its high cost and technical importance, plasma equipment is still largely designed empirically, with little help from computer simulation. Plasma process control is rudimentary. Optimization of plasma reactor operation, including adjustments to deal with increasingly stringent controls on plant emissions, is performed predominantly by trial and error. There is now a strong and growing economic incentive to improve on the traditional methods of plasma reactor and process design, optimization, and control. An obvious strategy for both chip manufacturers and plasma equipment suppliers is to employ large-scale modeling and simulation. The major roadblock to further development of this promising strategy is the lack of a database for the many physical and chemical processes that occur in the plasma. The data that are currently available are often scattered throughout the scientific literature, and assessments of their reliability are usually unavailable. Database Needs for Modeling and Simulation of Plasma Processing identifies strategies to add data to the existing database, to improve access to the database, and to assess the reliability of the available data. In addition to identifying the most important needs, this report assesses the experimental and theoretical/computational techniques that can be used, or must be developed, in order to begin to satisfy these needs.


Numerical Analysis of the Non-equilibrium Plasma Flow in the Gaseous Electronics Conference Reference Reactor*Project Supported by the National Natural Science Foundation of China (Nos. 11372325, 11475239).

Numerical Analysis of the Non-equilibrium Plasma Flow in the Gaseous Electronics Conference Reference Reactor*Project Supported by the National Natural Science Foundation of China (Nos. 11372325, 11475239).

Author:

Publisher:

Published: 2016

Total Pages:

ISBN-13:

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Abstract: The capacitively coupled plasma in the gaseous electronics conference reference reactor is numerically investigated for argon flow using a non-equilibrium plasma fluid model. The finite rate chemistry is adopted for the chemical non-equilibrium among species including neutral metastable, whereas a two-temperature model is employed to resolve the thermal non-equilibrium between electrons and heavy species. The predicted plasma density agrees very well with experimental data for the validation case. A strong thermal non-equilibrium is observed between heavy particles and electrons due to its low collision frequency, where the heavy species remains near ambient temperature for low pressure and low voltage conditions (0.1 Torr, 100 V). The effects of the operating parameters on the ion flux are also investigated, including the electrode voltage, chamber pressure, and gas flow rate. It is found that the ion flux can be increased by either elevating the electrode voltage or lowering the gas pressure.


An Experimental and Theoretical Study of the Non-equilibrium Plasma in Thermionic Discharges

An Experimental and Theoretical Study of the Non-equilibrium Plasma in Thermionic Discharges

Author: Ronald H. Curry

Publisher:

Published: 1967

Total Pages: 68

ISBN-13:

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Effective coefficients for ionization and radiative energy loss were computed for different values of electron temperature and density. These coefficients and the neutral density yield the rates for net ion production and radiative energy loss from all sources except the resonance lines. Energy loss from resonance lines and the ion production cost are considered separately. The following general conclusions can be drawn: (1) the area within 0.4 mm of the emitter is a source of ion-electron pairs, the rest of the plasma being a sink; (2) inelastic energy losses decrease monotonically from the emitter to the collector; and (3) these effects are relatively independent of cesium pressure, but are generally proportional to output density. Furthermore, the differential equations governing the transport of particles, momentum, and energy in the plasma between the electrodes of a thermionic converter were more completely formulated. Specific advances are the inclusion of more exact coefficients for electron transport and for ion production and radiative energy loss in the plasma volume. In diode experiments, the electron temperature was determined from measurement of the continuum emitted by radiative recombination to the 6P states of cesium, and the electron density was determined from Stark broadening of the fundamental series lines. Of particular interest is observation of forbidden lines. (Author).