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Many studies suggest that lean-NOx SCR proceeds via oxidation of NO to NO2 by oxygen, followed by the reaction of the NO2 with hydrocarbons. On catalysts that are not very effective in catalyzing the equilibration of NO+O2 and NO2, the rate of N2 formation is substantially higher when the input NOx is NO2 instead of NO. The apparent bifunctional mechanism in the SCR of NOx has prompted the use of mechanically mixed catalyst components, in which one component is used to accelerate the oxidation of NO to NO2, and another component catalyzes the reaction between NO2 and the hydrocarbon. Catalysts that previously were regarded as inactive for NOx reduction could therefore become efficient when mixed with an oxidation catalyst. Preconverting NO to NO2 opens the opportunity for a wider range of SCR catalysts and perhaps improves the durability of these catalysts. This paper describes the use of a non-thermal plasma as an efficient means for selective partial oxidation of NO to NO2.

In the effort to design reliable diesel engines which meet the strict US Federal Regulations for emissions, considerable progress has been made by engine manufacturers. Particulate emissions are now below 0.25 g/BHPh and after 1994 will be below 0.1 g/BHPh. Diesel fuel has a revised specification limit of 0.05% sulfur as a means to assist diesel engine manufacturers in complying with the 1994 standard. Diesel oxidation catalysts (DOC) have been chosen as another means. A DOC can efficiently oxidize soluble organic particulate matter (SOF) and gaseous hydrocarbons while easily oxidizing SO2 to SO3-the latter being a particulate and undesirable. Selective DOCs have been developed which maintain the activity for SOF and minimize the undesirable SO2 oxidation step. However, performance for gaseous hydrocarbons may be negatively affected.

This paper discusses the gas-phase reaction mechanisms for removal of NOx in a plasma. The effect of oxygen content on the competition between the reduction and oxidation processes is discussed. The effect of the electron kinetic energy distribution on the radical production and subsequent chemistry is then discussed in order to predict the best performance that can be achieved for NOx reduction using the plasma alone. The fundamental limit on the minimum electrical energy consumption that will be required to implement NOx reduction in any type of plasma reactor is established.

Plasma reactors can be operated as a particulate trap or as a NOx converter. Particulate trapping in a plasma reactor can be accomplished by electrostatic precipitation. The soluble organic fraction of the trapped particulates can be utilized for the hydrocarbon-enhanced oxidation of NO to NO2. The NO2 can then be used to non-thermally oxidize the carbon fraction of the particulates. The oxidation of the carbon fraction by NO2 can lead to reduction of NOx or backconversion of NO2 to NO. This paper examines the hydrocarbon and electrical energy density requirements in a plasma for maximum NOx conversion in both heavy-duty and light-duty diesel engine exhaust. The energy density required for complete oxidation of hydrocarbons is also examined and shown to be much greater than that required for maximum NOx conversion. The reaction of NO2 with carbon is shown to lead mainly to backconversion of NO2 to NO.

Mixing controlled compression ignition, i.e., diesel engines are efficient and are likely to continue to be the primary means for movement of goods for many years. Low-net-carbon biofuels have the potential to significantly reduce the carbon footprint of diesel combustion and could have advantageous properties for combustion, such as high cetane number and reduced engine-out particle and NOx emissions. We developed a list of over 400 potential biomass-derived diesel blendstocks and populated a database with the properties and characteristics of these materials. Fuel properties were determined by measurement, model prediction, or literature review. Screening criteria were developed to determine if a blendstock met the basic requirements for handling in the diesel distribution system and use as a blend with conventional diesel. Criteria included cetane number ≥40, flashpoint ≥52°C, and boiling point or T90 ≤338°C.

Recently, catalyzed soot filters (CSF) for passenger vehicles have been introduced into the marketplace to comply with the European environmental requirements and future emission standards. The initial system consisted of one or two diesel oxidation catalysts (DOC) to meet the regulated HC and CO standards along with an under floor CSF to treat the particulate emissions. In order to meet the cold start requirements and to reduce system costs with a CSF only unit, converters are placed closer to the engine to minimize heat losses and more of the DOC functionality is integrated into the filter substrate. This work describes the development of such DOC-integrated CSF systems. One major challenge in the design of such systems is to ensure that there is sufficient catalyst functionality within the wall-flow substrate while maintaining an acceptable exhaust gas backpressure across the filter.