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A dielectric barrier discharge device has been built to test nonthermal plasma discharges for simulated diesel exhaust NOx removal. The device has also been tested with selected catalysts located after the plasma. Emissions are measured by conventional automotive emission analyzers, plus FTIR. Dielectric barrier discharges without catalyst convert input NO to a mix of NO2, HONO, HNO3, and organic nitrates. At 30 J/l energy deposition, approximately 26% of the input NO is “lost”. Some of the hydrocarbon input is converted to a variety of species, including CO, CO2, aldehydes, and alcohols. A Cu-ZSM catalyst after the plasma device eliminates the apparent NOx conversion seen with the bare plasma. This indicates that the apparent NOx conversion of the bare plasma is actually conversion to some (unmeasured) species which can be reconverted to NOx by the Cu-ZSM catalyst. Placing a proprietary catalyst within the plasma results in significant NOx conversion.

There is a need for an efficient, durable technology to reduce NOx emissions from oxidative exhaust streams such as those produced by compression-ignition, direct-injection (CIDI) diesel or lean-burn gasoline engines. A partnership formed between the DOE Office of Advanced Automotive Technology, Pacific Northwest National Laboratory, Oak Ridge National Laboratory and the USCAR Low Emission Technologies Research and Development Partnership is evaluating the effectiveness of a non-thermal plasma in conjunction with catalytic materials to mediate NOx and particulate emissions from diesel fueled light duty (CIDI) engines. Preliminary studies showed that plasma-catalyst systems could reduce up to 70% of NOx emissions at an equivalent cost of 3.5% of the input fuel in simulated diesel exhaust. These studies also showed that the type and concentration of hydrocarbon play a key role in both the plasma gas phase chemistry and the catalyst surface chemistry.

We present data in this paper showing that non-thermal plasma in combination with heterogeneous catalysis is a promising technique for the treatment of NOx in diesel exhaust. Using a commonly available zeolite catalyst, sodium Y, to treat synthetic diesel exhaust we report approximately 50% chemical reduction of NOx over a broad, representative temperature range. We have measured the overall efficiency as a function of the temperature and hydrocarbon concentration. The direct detection of N2 and N2O when the background gas is replaced by helium confirms that true chemical reduction is occurring.