An official website of the United States government
Natural gas associated with oil wells and natural gas fields is a significant source of greenhouse gas emissions and airborne pollutants. Flaring of the associated gas removes greenhouse gases like methane and other hydrocarbons. The present study explores the possibility of enhancing the flaring of associated gas mixtures (C1 – C4 alkane mixture) using nanosecond pulsed non-equilibrium plasma discharges. Starting with a detailed chemistry for C0 – C4 hydrocarbons (Aramco mechanism 3.0 – 589 species), systematic reductions are performed to obtain a smaller reduced mechanism (156 species) yet retaining the relevant kinetics of C1 – C4 alkanes at atmospheric pressure and varying equivalence ratios (φ = 0.5 – 2.0). This conventional combustion chemistry for small alkanes is then coupled with the plasma kinetics of CH4, C2H6, C3H8, and N2, including electron-impact excitations, dissociations, and ionization reactions. The newly developed plasma-based flare gas chemistry is then utilized to investigate repetitively pulsed non-equilibrium plasma-assisted reforming and subsequent combustion of the flare gas mixture diluted with N2 at different conditions. The results indicate an enhanced production of hydrogen, ethylene and other species in the reformed gas mixture, owing to the electron-impact dissociation pathways and subsequent H-abstractions and recombination reactions, thereby resulting in a mixture of CH4, H2, C2H4, C2H2, and other unsaturated C3 species. The reformed mixture shows an enhanced reactivity as exhibited by their shorter ignition delays. The reformed mixture is also observed to undergo increased methane destruction and higher equilibrium temperatures compared to the original mixture as the gas temperature increases, thereby exhibiting a potential for reducing the unburnt emissions of methane and other hydrocarbons.
more »
« less
3D phenomenological modeling of plasma-assisted methane reforming
Natural gas contains a significant fraction of methane, a strong greenhouse gas besides being a potent hydrogen carrier. Thus, reforming methane to a more reactive gas mixture could potentially abate the associated greenhouse heating by depleting methane and provide a pathway to generate hydrogen. The present study investigates the non-equilibrium plasma-assisted reforming of methane to produce hydrogen and reactive alkenes using repetitive nanosecond pulse discharges. A detailed gas-phase chemical kinetics mechanism along with plasma reforming kinetics derived from our previous work are used to perform 0D calculations to obtain the energy fractions for various plasma processes. A phenomenological model for the plasma-assisted reforming of methane/nitrogen mixtures is developed by considering the vibrational energy transport equations of both methane and nitrogen separately. The energy fractions involved in various plasma processes, such as ultra-fast gas heating and ultra-fast gas dissociation due to the electron excitation reactions, and slow gas heating due to the relaxation of vibrational excitation modes of methane and nitrogen, are accounted for in our new phenomenological model using energy fractions derived earlier. The newly developed phenomenological model is then used to perform 3D direct numerical simulation (DNS) of methane reforming diluted with 60% nitrogen in a pin-to-pin electrode configuration with a discharge gap of 1 mm. The effect of pulsing on the evolution of reformed mixture kernels is investigated by comparing two cases: a single-pulsed case with a pulse energy of 0.8 mJ, and another case using 4 pulses at 200 kHz, with a per pulse energy of 0.2 mJ. The single-pulsed case was observed to promote kernel separation and higher fractions of reformed products, while the multiple-pulsed case resulted in a more diffused kernel.
more »
« less
- Award ID(s):
- 2002635
- PAR ID:
- 10562100
- Publisher / Repository:
- American Institute of Aeronautics and Astronautics
- Date Published:
- ISBN:
- 978-1-62410-711-5
- Page Range / eLocation ID:
- AIAA 2024-0403
- Format(s):
- Medium: X
- Location:
- Orlando, FL
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
This work aims at comparing the accuracy and overall performance of a low-Mach CFD solver and a fully-compressible CFD solver for direct numerical simulation (DNS) of nonequilibrium plasma assisted ignition (PAI) using a phenomenological model described in Castela et al. [1]. The phenomenological model describes the impact of nanosecond pulsed plasma discharges by introducing source terms in the reacting flow equations, instead of solving the detailed plasma kinetics at every time step of the discharge. Ultra-fast gas heating and dissociation ofO2 are attributed to the electronic excitation ofN2 and the subsequent quenching to ground state. This process is highly exothermic, and is responsible for dissociation of O2 to form O radicals; both of which promote faster ignition. Another relatively slower process of gas heating associated with vibrational-to-translational relaxation is also accounted for, by solving an additional vibrational energy transport equation. A fully-compressible CFD solver for high Mach (M>0.2) reacting flows, developed by extending the default rhoCentralFoam solver in OpenFOAM, is used to perform DNS of PAI in a 2D domain representing a cross section of a pin-to-pin plasma discharge configuration. The same case is also simulated using a low-Mach, pressure-based CFD solver, built by extending the default reactingFoam solver. The lack of flow or wave dominated transport after the plasma-induced weak shock wave leaves the domain causes inaccurate computation of all the transport variables, with a rather small time step dictated by the CFL condition, with the fully-compressible solver. These issues are not encountered in the low-Mach solver. Finally, the low-Mach solver is used to perform DNS of PAI in lean, premixed, isotropic turbulent mixtures of CH4-air at two different Reynolds numbers of 44 and 395. Local convection of the radicals and vibrational energy from the discharge domain, and straining of the high temperature reaction zones resulted in slower ignition of the case with the higher Re. A cascade effect of temperature reduction in the more turbulent case also resulted in a five - six times smaller value of the vibrational to translational gas heating source term, which further inhibited ignition. Two pulses were sufficient for ignition of the Re = 44 case, whereas three pulses were required for the Re = 395 case; consistent with the results of Ref. [1].more » « less
-
Nanosecond Pulsed High Frequency Discharges (NPHFD) are gaining popularity over conventional spark and arc discharges as they have been shown to increase energy efficiency, enhance ignition probability and sustained kernel growth, and offer more flexibility and control for ignition applications under various conditions. Hence, it is important to determine the impact of different factors such as the optimal pulse energy, background flow conditions, inter-pulse time, mixture equivalence ratio, etc. on the success of ignition of premixed mixtures with NPHFD. This work presents a numerical investigation of the morphology of ignition kernel development with both single-pulse and multiple-pulse discharges. Nanosecond non-equilibrium plasma discharges are modeled between pin-pin electrodes in a subsonic ignition tunnel with quiescent and flowing premixed mixtures of methane and air. Large eddy simulations (LES) are conducted to investigate the reasons for successful and failed ignition in different scenarios. A single pulse discharge in the presence of electrodes, in a quiescent medium, elucidates the gas recirculation pattern caused by the plasma pulse which results in a separated toroidal kernel from the primary ignition kernel between the electrodes. Convection heat loss to the mean flow results in quenching of the high temperature, radical-rich hot-spots creeping on the electrode walls, and leaving only the semi-toroidal kernel to propagate downstream. Finally, simulations with multiple pulses with different inter-pulse times have been conducted to analyze the synergistic effect of overlapping kernels with high temperature and OH concentration, which has been attributed as the primary reason for higher ignition probabilities in the “fully coupled” regime reported in the experiments. Successful ignition kernel formation is reported with 3 pulses at a pulse repetition frequency of 300 kHz in the fully coupled regime. This kernel volume was almost 4 times, and develops in two-thirds the time, compared to the ignition kernel volume formed by the single pulse discharge with the same total energy. Ten pulses with twice as much total energy were deposited at a much lower frequency of 2 kHz, which resulted in disjoint hot-spots that fail to form an ignition kernel in the decoupled regime.more » « less
-
Nanosecond pulsed plasmas have been demonstrated, both experimentally and numerically, to be beneficial for ignition, mainly through gas heating (at different timescales) and radical seeding. However, most studies focus on specific gas conditions, and little work has been done to understand how plasma performance is affected by fuel and oxygen content, at different gas temperatures and deposited energies. This is relevant to map the performance envelope of plasma-assisted combustion across different regimes, spanning from fuel-lean to fuel-rich operation, as well as oxygen-rich to oxygen-vitiated conditions, of interest to different industries. This work presents a computational effort to address a large parametric exploration of combustion environments and map out the actuation authority of plasmas under different conditions. The work uses a zero-dimensional plasma-combustion kinetics solver developed in-house to study the ignition of CH4/O2/N2 mixtures with plasma assistance. A main contribution of the study is the detailed tracking of the energy, from the electrical input all the way to the thermal and kinetic effects that result in combustion enhancement. This extends prior works that focus on the first step of the energy transfer: from the electrical input to the electron-impact processes. Independent of the composition, four pathways stand out: (i) vibrational-translational relaxation, (ii) fast gas heating, (iii) O2 dissociation, and (iv) CH4 dissociation. Results show that the activated energy pathways are highly dependent on gas state, composition, and pulse shape, and can explain the observed range in performance regarding ignition enhancement. The approach can be used to calculate the fractional energy deposition into the main pathways for any mixture or composition, including new fuels, and can be a valuable tool to construct phenomenological models of the plasma across combustion environments.more » « less
-
Pepiot, Perrine (Ed.)The Global Pathway Analysis (GPA) algorithm helps analyze the chemical kinetics of complex combustion systems by identifying important global reaction pathways connecting a source species to a sink species through various important intermediate species (i.e., hub species). The present work aims to extend GPA algorithm to plasma-assisted combustion and fuel reforming systems to identify the dominant global pathways in such systems at various conditions. In addition, the present study extends the ability of GPA algorithm to identify reaction cycles involving the excitation of high-concentration species (e.g., O2, N2, and fuel) to their vibrational and electronic states and the subsequent de-excitation to their ground state, based on their significance on the reactivity of plasma-assisted systems in terms of gas heating and radical production. Provisions are made in the GPA algorithm to evaluate the reactivity of identified reaction pathways and cycles based on the element-flux transfer (i.e., dominance), heat release, and radical production rate. The newly developed Plasma-based Global Pathway Analysis (PGPA) algorithm is then used to analyze the plasma-assisted combustion of ammonia and reforming of methane. The PGPA analyses elucidated the significance of vibrational-translational cycles on the reactivity of NH3/air mixtures. Further, analyses on the production of NO ascribed the early reforming of NH3 to N2 and H2 in impeding the production of NO during plasma-assisted NH3 ignition. Lastly, the enhanced reforming of CH4/N2 mixtures using plasma has been attributed to electron impact dissociation of CH4 when compared to thermal reforming. In contrast, conventional path-Flux analysis (PFA) was found to require significant manual effort and pre-analysis intuitions from expert knowledge, making it arduous to provide valuable insights into plasma chemistry. The user-friendly and automated nature of PGPA thus provides a valuable tool for assessing the kinetics of plasma-assisted systems helpful in analyzing and, further, a foundation in reducing plasma-assisted chemistry, without the needs of expert knowledge.more » « less
- Free Publicly Accessible Full Text
-
Accepted Manuscript1.0
- Conference Paper:
- https://doi.org/10.2514/6.2024-0403
