Low- and intermediate-temperature ammonia/hydrogen oxidation in a flow reactor: Experiments and a wide-range kinetic modeling

Abstract

Understanding the chemistry behind the oxidation of ammonia/hydrogen mixtures is crucial for ensuring the flexible use of such mixtures in several applications, related to propulsion systems and power generation. In this work, the oxidation of ammonia/hydrogen blends was investigated through an experimental and kinetic-modeling study, where the low- and intermediate-temperature conditions were considered. An experimental campaign was performed in a flow reactor, at stoichiometric conditions and near-atmospheric pressure (126.7 kPa). The mole fraction of fuels, oxidizer and final products was measured. At the same time, a comprehensive kinetic model was set up, following a modular and hierarchical approach, and implementing the recently-available elementary rates. Such a model was used to interpret the experimental results, and to extend the analysis to literature data, covering several oxidation features. The reactivity boost provided by H2 addition was found to be approximately linear with its mole fraction in both flow- and jet-stirred-reactor conditions (except for the smallest H2 amounts in the flow reactor), in contrast with the more-than-linear increase in the laminar flame speed. The key role of HO2 in regulating fuel conversion and autoignition at low temperature was confirmed for binary mixtures, with H2NO being the bottleneck to the low-temperature oxidation of NH3-rich blends. On the other hand, the nitrogen fate was found to be mostly regulated by NHx + NO propagation and termination channels.