Sulfur Tolerance of Selective Partial Oxidation of NO to NO2 in a Plasma

Several catalytic aftertreatment technologies rely on the conversion of NO to NO2 to achieve efficient reduction of NOx and particulates in diesel exhaust. These technologies include the use of selective catalytic reduction of NOx with hydrocarbons, NOx adsorption, and continuously regenerated particulate trapping. These technologies require low sulfur fuel because the catalyst component that is active in converting NO to NO2 is also active in converting SO2 to SO3 . The SO3 leads t o increase in particulates and/or poison active sites on the catalyst. A non-thermal plasma can be used for the selective partial oxidation of NO to NO2 in the gas-phase under diesel engine exhaust conditions. This paper discusses how a non-thermal plasma can efficiently oxidize NO to NO2 without oxidizing SO2 to SO3

Flash X-Ray (FXR) Accelerator Optimization Beam-Induced Voltage Simulation and TDR Measurements

Lawrence Livermore National Laboratory (LLNL) is evaluating design alternatives to improve the voltage regulation in our Flash X-Ray (FXR) accelerator cell and pulse-power system. The goal is to create a more mono-energetic electron beam. When an electron beam crosses the energized gap of an accelerator cell, the electron energy is increased. However, the beam with the associated electromagnetic wave also looses a small amount of energy because of the increased impedance seen across the gap. The beam-induced voltage at the gap is time varying. This creates beam energy variations that we need to understand and control. A high-fidelity computer simulation of the beam and cell interaction has been completed to quantify the time varying induced voltage at the gap. The cell and pulse-power system was characterized using a Time-domain Reflectometry (TDR) measurement technique with a coaxial air-line to drive the cell gap. The beam-induced cell voltage is computed by convoluting the cell impedance with measured beam current. The voltage was checked against other measurements to validate the accuracy

Final report pulsed plasma processing of effluent pollutants and hazardous chemicals

The electrical discharge techniques, called non-thermal, utilize high voltage breakdown of gases using short pulses of one to a few hundred nanoseconds. These short pulses between metal electrodes generate energetic electrons without appreciable thermal heating of the gas. The energetic electrons collide with gas molecules to form radicals. The radicals then react with pollutants to form harmless compounds. Our non-thermal experimental device used a wire in a pipe geometry. The wire was driven by a 40 kilovolt pulse 100 nanoseconds long. Gas was circulated in a loop through the pipe geometry in a closed system. This system permitted the introduction of various gas combinations prior to testing. The recirculated gas was heated to determine the effect on the electrical discharge, and chemical reactions. Additives were introduced to improve the efficiency (defined as energy input per unit molecule destroyed). The efficient was found to be the most important parameter in that the experiments generally required high energy inputs. However, we were able to significantly improve the efficiency of NO removal by the addition of hydrocarbons, nitric oxide has been removed with an energy cost of 15 ev per NO molecule. We believe the hydrocarbon additive serves by recycling the hydroxyl radicals during the oxidation of NO. The implementation of this process will depend largely on how much additives, electrical power consumption, and final NO{sub x} concentration are acceptable for a particular application

Fundamental limits on chemical reduction of NO{sub x} by non-thermal plasmas

The objective of this paper is to establish the fundamental limits on the minimum electrical energy consumption that will be required to implement true chemical reduction of NOx by the plasma alone. The effect of background gas composition particularly the oxygen content on the completion between the reduction and oxidation processes will be discussed. The effect of the electron kinetic energy distribution on the radical production and subsequent chemistry will also be discussed

Plasma Aftertreatment for Simultaneous Control of NOx and Particulates

Plasma reactors can be operated as a particulate trap or as a NO{sub x} converter. The soluble organic fraction (SOF) of the trapped particulates can be utilized for the oxidation of NO to NO{sub 2}. The NO{sub 2} can then be used to non-thermally oxidize the carbon fraction of the particulates. This paper examines the energy density required for oxidation of the SOF hydrocarbons and the fate of NO{sub 2} during the oxidation of the particulate carbon. The energy density required for complete oxidation of the SOF hydrocarbons is shown to be unacceptably large. The reaction of NO{sub 2} with carbon is shown to lead mainly to backconversion of NO{sub 2} to NO. These results suggest that the use of a catalyst in combination with the plasma will be required to efficiently reduce the NO{sub x} and oxidize the SOF hydrocarbons

Study of Vacuum Insulator Flashover for Pulse Lengths of Multi-Microseconds

We are studying the flashover of vacuum insulators for applications where high voltage conditioning of the insulator and electrodes is not practical and for pulse lengths on the order of several microseconds. The study is centered about experiments performed with a 100-kV, 10-ms pulsed power system and supported by a combination of theoretical and computational modeling. The base line geometry is a cylindrically symmetric, +45{sup o} insulator between flat electrodes. In the experiments, flashovers or breakdowns are localized by operating at field stresses slightly below the level needed for explosive emissions with the base line geometry. The electrodes and/or insulator are then seeded with an emission source, e.g. a tuft of velvet, or a known mechanical defect. Various standard techniques are employed to suppress cathode-originating flashovers/breakdowns. We present the results of our experiments and discuss the capabilities of modeling insulator flashover

Basic energy efficiency of plasma production in electrical discharge and electron beam reactors

Non-thermal plasma processing is an emerging technology for the abatement of volatile organic compounds (VOCs) and nitrogen oxides (NO{sub x}) in atmospheric pressure gas streams. Either electrical discharge of electron beam methods can produce these plasmas. This paper presents a comparative assessment of various non-thermal plasma reactors. The goal of our project is two-fold: (1) to understand the feasibility and scalability of various non-thermal plasma reactors by focusing on the energy efficiency of the electron and chemical kinetics, and (2) to optimize process parameters and provide performance and economic data. Experimental results using a compact electron beam reactor, pulsed corona reactor and dielectric-barrier discharge will be presented. These reactors have been used to study the removal of NO{sub x} and a wide variety of VOCs. The effects of background gas decomposition and gas temperature on the decomposition chemistry have been studied. The decomposition mechanisms are discussed to illustrate how the chemistry could strongly affect the economics of the process. An analysis of the electron kinetics show that electrical discharge reactors are the most suitable only for processes requiring O radicals. For pollution control applications requiring copious amounts of electrons, ions, N atoms or OH radicals, the sue of electron beam reactors is generally the best way of minimizing the electrical power consumption

Nonthermal aftertreatment of diesel engine exhaust

The ultimate objective of this work has been to develop a nonthermal plasma process to reduce NO{sub x} in diesel exhaust gas. A secondary objective has been to study the possibility of particulate matter (soot) reduction by the same technique. The early work revealed a fundamental difficulty with this NO{sub x} reduction approach in the gas environment of the diesel engine exhaust. These observations necessitated a thorough study of the unfavorable chemistry in the hope that knowledge of the chemical mechanism would offer an opportunity to make the approach useful for NO{sub x} reduction. Whereas fundamental understanding of the mechanism has been obtained, the authors have not found any measure that would make the approach meet its original objective

Flash X-Ray (Fxr) Linear Induction Accelerator (Lia) Optimization Sensor Delay Correction

The radiographic goal of the FXR Optimization Project is to generate an x-ray pulse with peak energy of 19 MeV, spot-size of 1.5 mm, a dose of 500 rad, and duration of 60 ns. The electrical objectives are to generate a 3 kA electron-beam and refine our 16 MV accelerator so that the voltage does not vary more than 1%-rms. In a multi-cell linear induction accelerator, like FXR, the timing of the acceleration pulses relative to the beam is critical. The pulses must be timed optimally so that a cell is at full voltage before the beam arrives and does not drop until the beam passes. In order to stay within the energy-variation budget, the synchronization between the cells and beam arrival must be controlled to a couple of nanoseconds. Therefore, temporal measurements must be accurate to a fraction of a nanosecond. FXR Optimization Project developed a one-giga-sample per second (gs/s) data acquisition system to record beam sensor data. Signal processing algorithms were written to determine cell timing with an uncertainty of a fraction of a nanosecond. However, the uncertainty in the sensor delay was still a few nanoseconds. This error had to be reduced if we are to improve the quality of the electron beam. Two types of sensors are used to align the cell voltage pulse against the beam current. The beam current is measured with resistive-wall sensors. The cell voltages are read with capacitive voltage monitors. Sensor delays can be traced to two mechanisms: (1) the sensors are not co-located at the beam and cell interaction points, and (2) the sensors have different length jumper cables and other components that connect them to the standard-length coaxial cables of the data acquisition system. Using the physical locations and dimensions of the sensor components, and the dielectric constant of the materials, delay times were computed. Relative to the cell voltage, the beam current was theoretically reporting late by 7.7 ns. Two experiments were performed to verify and refine the sensor delay correction. In the first experiment, the beam was allowed to drift through a cell that was not pulsed. The beam induces a potential into the cell that is read by the voltage monitor. Analysis of the data indicated that the beam sensor signal was likely 7.1 ns late. In the second experiment, the beam current is calculated from the injector diode voltage that is the sum of the cell voltages. A 7 ns correction produced a very good match between the signals from the two types of sensors. For simplicity, we selected a correction factor that advanced the current signals by 7 ns. This should reduce the uncertainty in the temporal measurements to less than 1 ns

Understanding and Improving High Voltage Vacuum Insulators for Microsecond Pulses

High voltage insulation is one of the main areas of pulsed power research and development, and dielectric breakdown is usually the limiting factor in attaining the highest possible performance in pulsed power devices. For many applications the delivery of pulsed power into a vacuum region is the most critical aspect of operation. The surface of an insulator exposed to vacuum can fail electrically at an applied field more than an order or magnitude below the bulk dielectric strength of the insulator. This mode of breakdown, called surface flashover, imposes serious limitations on the power flow into a vacuum region. This is especially troublesome for applications where high voltage conditioning of the insulator and electrodes is not practical and for applications where relatively long pulses, on the order of several microseconds, are required. The goal of this project is to establish a sound fundamental understanding of the mechanisms that lead to surface flashover, and then evaluate the most promising techniques to improve vacuum insulators and enable high voltage operation at stress levels near the intrinsic bulk breakdown limits of the material. The approach we proposed and followed was to develop this understanding through a combination of theoretical and computation methods coupled with experiments to validate and quantify expected behaviors. In this report we summarize our modeling and simulation efforts, theoretical studies, and experimental investigations. The computational work began by exploring the limits of commercially available codes and demonstrating methods to examine field enhancements and defect mechanisms at microscopic levels. Plasma simulations with particle codes used in conjunction with circuit models of the experimental apparatus enabled comparisons with experimental measurements. The large scale plasma (LSP) particle-in-cell (PIC) code was run on multiprocessor platforms and used to simulate expanding plasma conditions in vacuum gap regions. Algorithms were incorporated into LSP to handle secondary electron emission from dielectric materials to enable detailed simulations of flashover phenomenon. Theoretical studies were focused on explaining a possible mechanism for anode initiated surface flashover that involves an electron avalanche process starting near the anode, not a mechanism involving bulk dielectric breakdown. Experiments were performed in Engineering's Pulsed Power Lab using an available 100-kV, 10-{micro}s pulse generator and vacuum chamber. The initial experiments were done with polyethylene insulator material in the shape of a truncated cone cut at +45{sup o} angle between flat electrodes with a gap of 1.0 cm. The insulator was sized so there were no flashovers or breakdowns under nominal operating conditions. Insulator flashover or gap closure was induced by introducing a plasma source, a tuft of velvet, in proximity to the insulator or electrode