Lawrence Berkeley National Laboratory

Ammonia often occurs in combustion gases as a product of fuel-nitrogen. Since either NO or N2 may predominate as the product of ammonia oxidation, there is considerable interest in understanding the factors responsible for selecting the final products. In flames the selectivity is known to depend on whether the reaction zones are premixed or non-premixed. This paper reports on a combined experimental and modeling investigation of ammonia chemistry in a hot combustion environment that is below flame temperatures, such as in post combustion gases. Experiments that mix highly diluted ammonia-methane and oxygen-water streams are interpreted in terms of a plug-flow model, a simplified mixing reactor model, and a two-dimensional direct numerical simulation. The study finds that the final products of ammonia oxidation remain sensitive to mixing even at temperatures below those of self-sustaining flames. At low temperatures ammonia oxidation occurs in a premixed reaction zone, but at sufficiently high temperatures a nonpremixed reaction zone may develop that produces significantly less NO than the equivalent premixed system. A direct numerical simulation is required to predict the behavior over the full range of conditions investigated experimentally, while a simplified reactor model captures the essential features as long as the radial gradients are not too steep.