Minimizing the impacts of the ammonia economy on the nitrogen cycle and climate.

Ammonia (NH3) is an attractive low-carbon fuel and hydrogen carrier. However, losses and inefficiencies across the value chain could result in reactive nitrogen emissions (NH3, NOx, and N2O), negatively impacting air quality, the environment, human health, and climate. A relatively robust ammonia economy (30 EJ/y) could perturb the global nitrogen cycle by up to 65 Mt/y with a 5% nitrogen loss rate, equivalent to 50% of the current global perturbation caused by fertilizers. Moreover, the emission rate of nitrous oxide (N2O), a potent greenhouse gas and ozone-depleting molecule, determines whether ammonia combustion has a greenhouse footprint comparable to renewable energy sources or higher than coal (100 to 1,400 gCO2e/kWh). The success of the ammonia economy hence hinges on adopting optimal practices and technologies that minimize reactive nitrogen emissions. We discuss how this constraint should be included in the ongoing broad engineering research to reduce environmental concerns and prevent the lock-in of high-leakage practices.

Finite flame thickness effects on Kolmogorov-Petrovsky-Piskunov turbulent burning velocities.

KPP (Kolmogorov-Petrovsky-Piskunov) solutions of the reaction-diffusion equation have application in various physical phenomena occurring in biology, ecology, and reacting flows. In particular, these solutions are commonly used in turbulent combustion to scale turbulent burning velocities. Subject to certain conditions on reaction rate profile through the flame brush and turbulent diffusivity, this theory relates the turbulent burning velocity to the derivative of the reaction rate (ω[over ̃]) at the leading edge of the flame brush (dω[over ̃]/dc[over ̃]|_{c[over ̃]=0}). Such waves are often referred to as "pulled fronts." However, turbulent flames never actually satisfy the KPP conditions for a pulled front, as the turbulent flame brush, parametrized here by the thickness δ_{t}, consists of an ensemble of laminar flamelets of thickness δ, where ε=δ/δ_{t}≪1 is very small, but nonzero, and dω[over ̃]/dc[over ̃] tends to zero at the brush leading edge for high activation energy, combustion-type kinetics. This paper analyzes these effects on KPP wave solutions, parametrized by ε=δ/δ_{t} and Zeldovich number Ze focusing on whether turbulent flames retain their pulled front character and what the correction to the KPP wave speed is. Variational solutions of the reaction-diffusion equation show that the solution can be expanded in powers of 1/|lnε|. Both numerical and asymptotic results are presented, showing that the wave still exhibits pulled front solutions but with significant corrections to the KPP result. The leading order correction is of the form |lnε|^{-2} and independent of Ze. Higher order corrections are function of both ε and Ze. However, the dominant factor influencing the wave speed correction is due to the finite ε, with Ze exhibiting a weaker effect.

Characterization of forced response of density stratified reacting wake.

The hydrodynamic stability of a reacting wake depends primarily on the density ratio [i.e., ratio of unburnt gas density (ρu) to burnt gas density (ρb)] of the flow across the wake. The variation of the density ratio from high to low value, keeping ρu/ρb>1, transitions dynamical characteristics of the reacting wake from a linearly globally stable (or convectively unstable) to a globally unstable mode. In this paper, we propose a framework to analyze the effect of harmonic forcing on the deterministic and synchronization characteristics of reacting wakes. Using the recurrence quantification analysis of the forced wake response, we show that the deterministic behaviour of the reacting wake increases as the amplitude of forcing is increased. Furthermore, for different density ratios, we found that the synchronization of the top and bottom branches of the wake with the forcing signal is dependent on whether the mean frequency of the natural oscillations of the wake (fn) is lesser or greater than the frequency of external forcing (ff). We notice that the response of both branches (top and bottom) of the reacting wake to the external forcing is asymmetric and symmetric for the low and high density ratios, respectively. Furthermore, we characterize the phase-locking behaviour between the top and bottom branches of the wake for different values of density ratios. We observe that an increase in the density ratio results in a gradual decrease in the relative phase angle between the top and bottom branches of the wake, which leads to a change in the vortex shedding pattern from a sinuous (anti-phase) to a varicose (in-phase) mode of the oscillations.

Nonlinear dynamics and intermittency in a turbulent reacting wake with density ratio as bifurcation parameter.

The flame or flow behavior of a turbulent reacting wake is known to be fundamentally different at high and low values of flame density ratio (ρ_{u}/ρ_{b}), as the flow transitions from globally stable to unstable. This paper analyzes the nonlinear dynamics present in a bluff-body stabilized flame, and identifies the transition characteristics in the wake as ρ_{u}/ρ_{b} is varied over a Reynolds number (based on the bluff-body lip velocity) range of 1000-3300. Recurrence quantification analysis (RQA) of the experimentally obtained time series of the flame edge fluctuations reveals that the time series is highly aperiodic at high values of ρ_{u}/ρ_{b} and transitions to increasingly correlated or nearly periodic behavior at low values. From the RQA of the transverse velocity time series, we observe that periodicity in the flame oscillations are related to periodicity in the flow. Therefore, we hypothesize that this transition from aperiodic to nearly periodic behavior in the flame edge time series is a manifestation of the transition in the flow from globally stable, convective instability to global instability as ρ_{u}/ρ_{b} decreases. The recurrence analysis further reveals that the transition in periodicity is not a sudden shift; rather it occurs through an intermittent regime present at low and intermediate ρ_{u}/ρ_{b}. During intermittency, the flow behavior switches between aperiodic oscillations, reminiscent of a globally stable, convective instability, and periodic oscillations, reminiscent of a global instability. Analysis of the distribution of the lengths of the periodic regions in the intermittent time series and the first return map indicate the presence of type-II intermittency.

Acoustic near-field characteristics of a conical, premixed flame.

The occurrence of self-excited pressure oscillations routinely plagues the development of combustion systems. These oscillations are often driven by interactions between the flame and acoustic perturbations. This study was performed to characterize the structure of the acoustic field in the near field of the flame and the manner in which it is influenced by oscillation frequency, combustor geometry, flame length and temperature ratio. The results of these calculations indicate that the acoustic velocity has primarily one- and two-dimensional features near the flame tip and base, respectively. The magnitude of the radial velocity components increases with temperature ratio across the flame, while their axial extent increases with frequency. However, the acoustic pressure has primarily one-dimensional characteristics. They also show that the acoustic field structure exhibits only moderate dependencies upon area expansion and flame temperature ratio for values typical of practical systems. Finally, they show that the local characteristics of the acoustic field, as well as the overall plane-wave reflection coefficient, exhibit a decreasing dependence upon the flame length as the area expansion ratio increases.