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At least 109 records · Page 6

A Process-based, Climate-Sensitive Model to Derive Methane Emissions from Natural Wetlands: Application to 5 Wetland Sites, Sensitivity to Model Parameters and Climate

Methane emissions from natural wetlands constitutes the largest methane source at present and depends highly on the climate. In order to investigate the response of methane emissions from natural wetlands to climate variations, a 1-dimensional process-based climate-sensitive model to derive methane emissions from natural wetlands is developed. In the model the processes leading to methane emission are simulated within a 1-dimensional soil column and the three different transport mechanisms diffusion, plant-mediated transport and ebullition are modeled explicitly. The model forcing consists of daily values of soil temperature, water table and Net Primary Productivity, and at permafrost sites the thaw depth is included. The methane model is tested using observational data obtained at 5 wetland sites located in North America, Europe and Central America, representing a large variety of environmental conditions. It can be shown that in most cases seasonal variations in methane emissions can be explained by the combined effect of changes in soil temperature and the position of the water table. Our results also show that a process-based approach is needed, because there is no simple relationship between these controlling factors and methane emissions that applies to a variety of wetland sites. The sensitivity of the model to the choice of key model parameters is tested and further sensitivity tests are performed to demonstrate how methane emissions from wetlands respond to climate variations.

Walter, Bernadette P.↗

The mechanisms of flame holding in the wake of a bluff body

The flame holding mechanism for lean methane- and lean propane-air flames is examined under conditions where the recirculation zone is absent. The main objective of this work is to study the holding process in detail in an attempt to determine the mechanism of flame holding and also the conditions where this mechanism is viable and when it fails and blow-off occurs. Inverted flames held in the wake of a flat strip were studied. Experiments with different sizes of flame holders were performed. The velocity flow field was determined using a laser Doppler velocimetry technique. Equation of continuity was used to calculate the flame temperature from the change in area of flow streamlines before and after the flame. Observations of the inverted flame itself were obtained using schlieren and direct photography. Results show that there are different mechanisms operative at the time of blow-off for lean propane and methane flames. Blow-off or extinction occurs for lean propane-air flame in spite of the reaction going to completion and the disparity between the heat loss and the gain in mass diffusion in the reaction zone i.e., Le 1.0 causes the flame to blow-off. For methane-air flame the controlling factor or blow-off is incomplete reaction due to higher blowing rate leading to reduced residence time in the reaction zone.

Strehlow, R. A.↗

Methane emissions to the atmosphere through aquatic plants

The movement of methane (CH4) from anaerobic sediments through the leaves, stems, and flowers of aquatic plants and into the atmosphere was found to provide a significant pathway for the emission of CH4 from the aquatic substrates of flooded wetlands. Methane concentrations well above the surrounding ambient air levels were found in the mesophyll of 16 varies of aquatic plants and are attributed to transpiration, diffusion, and pressure-induced flow of gaseous CH4 from the roots when they are embedded in CH4-saturated anaerobic sediments. Methane emissions from the emergent parts of aquatic plants were measured using floating chamber techniques and by enclosing the plants in polyethylene bags of known volume. Concentration changes were monitored in the trapped air using syringes and gas chromatographic techniques. Vertical profiles of dissolved CH4 in sediment pore water surrounding the aquatic plants' rhizomes were obtained using an interstitial sampling technique. Methane emissions from the aquatic plants studied varied from 14.8 mg CH4/d to levels too low to be detectable. Rooted and unrooted freshwater aquatic plants were studied as well as saltwater and brackish water plants. Included in the experiment is detailed set of measurements on CH4 emissions from the common cattail (Typha latifolia). This paper illustrates that aquatic plants play an important gas exchange role in the C cycle between wetlands and the atmosphere.

Sebacher, D. I.↗

Turbulent Jet Flames Into a Vitiated Coflow

Examined is the vitiated coflow flame, an experimental condition that decouples the combustion processes of flows found in practical combustors from the associated recirculating fluid mechanics. The configuration consists of a 4.57 mm diameter fuel jet into a coaxial flow of hot combustion products from a lean premixed flame. The 210 mm diameter coflow isolates the jet flame from the cool ambient, providing a hot environment similar to the operating conditions of advanced combustors; this important high temperature element is lacking in the traditional laboratory experiments of jet flames into cool (room) air. A family of flows of increasing complexity is presented: 1) nonreacting flow, 2) all hydrogen flame (fuel jet and premixed coflow), and 3) set of methane flames. This sequence of experiments provides a convenient ordering of validation data for combustion models. Laser Raman-Rayleigh-LIF diagnostics at the Turbulent Diffusion Flame laboratory of Sandia National Laboratories produced instantaneous multiscalar point measurements. These results attest to the attractive features of the vitiated coflow burner and the well-defined boundary conditions provided by the coflow. The coflow is uniform and steady, isolating the jet flame from the laboratory air for a downstream distance ranging from z/d = 50-70. The statistical results show that differential diffusion effects in this highly turbulent flow are negligible. Complementing the comprehensive set of multiscalar measurements is a parametric study of lifted methane flames that was conducted to analyze flame sensitivity to jet and coflow velocity, as well as coflow temperature. The linear relationship found between the lift-off height and the jet velocity is consistent with previous experiments. New linear sensitivities were found correlating the lift-off height to coflow velocity and temperature. A blow-off study revealed that the methane flame blows off at a common coflow temperature (1260 K), regardless of coflow or jet velocity. An explanation for this phenomenon is that entrainment of ambient air at the high lift-off heights prevents autoignition. Analysis of the results suggests that flame stabilization occurs through a combination of flame propagation, autoignition, and localized extinction processes. Proposed is an expanded view of distributed reaction combustion based on analysis of the distributions of probe volume conditions at the stabilization region of the lifted hydrogen and methane flames. Turbulent eddies the size of the flame thickness mix fuel and hot coflow across the flame front, thereby enhancing the reaction zone with autoignition of reactants at elevated temperatures; this is the reverse effect of turbulent flames in ambient air, where intense turbulence in cool mixtures result in localized extinction. Each of the three processes (i.e., flame propagation, autoignition and localized extinction) contributes to flame stabilization in varying degrees, depending on flow conditions.

Holdeman, James D.↗

Confined Ni-In intermetallic alloy nanocatalyst with excellent coking resistance for methane dry reforming

Carbon dioxide and methane are two main greenhouse gases which are contributed to serious global warming. Fortunately, dry reforming of methane (DRM), a very important reaction developed decades ago, can convert these two major greenhouse gases into value-added syngas or hydrogen. The main problem retarding its industrialization is the seriously coking formation upon the nickel-based catalysts. Herein, a series of confined indium-nickel (In-Ni) intermetallic alloy nanocatalysts (In x Ni@SiO 2 ) have been prepared and displayed superior coking resistance for DRM reaction. The sample containing 0.5 wt.% of In loading (In 0.5 Ni@SiO 2 ) shows the best balance of carbon deposition resistance and DRM reactivity even after 430 h long term stability test. The boosted carbon resistance can be ascribed to the confinement of core–shell structure and to the transfer of electrons from Indium to Nickel in In-Ni intermetallic alloys due to the smaller electronegativity of In. Additionally, both the silica shell and the increase of electron cloud density on metallic Ni can weaken the ability of Ni to activate C–H bond and decrease the deep cracking process of methane. The reaction over the confined InNi intermetallic alloy nanocatalyst was conformed to the Langmuir-Hinshelwood (L-H) mechanism revealed by in situ diffuse reflectance infrared Fourier transform spectroscopy (in-situ DRIFTS). This work provides a guidance to design high performance coking resistance catalysts for methane dry reforming to efficiently utilize these two main greenhouse gases.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Effects of preferential diffusion on the burning intensity of curved flames

Using the Bunsen flame as a model curved flame, the coupled influence of preferential diffusion and flame stretch on the burning intensity of lean and rich mixtures of methane, propane, butane, ethylene, and hydrogen with air has been experimentally studied. The results substantiate theoretical predictions and quantify previous experimental observations that, for mixtures whose effective Lewis numbers (Le) are less than unity, the flame temperature is less than the adiabatic flame temperature. This temperature also decreases towards the flame tip, which has the largest curvature and therefore may locally extinguish. The dominance of diffusional transport in influencing the intensity of curved flames is demonstrated by showing that the tip opening of the highly diffusive hydrogen/air flames occurs at constant hydrogen equivalence ratios of about 1.15 to 1.20, being almost independent of the flow intensity and uniformity.

Mizomoto, M.↗

Carbon flux measurements from chambers collected between July to October 2022 at Old Woman Creek, Huron, Ohio.

This dataset contains carbon dioxide and methane flux measurements collected via chamber sampling at Old Woman Creek National Estuarine Research Reserve in Huron, OH. These data were generated to understand temporal and vegetation patterns associated with wetland carbon cycling. Specifically, this dataset intends to answer how carbon dioxide and methane fluxes change monthly and hourly across sites with vegetation and without vegetation. Data includes chamber measurements that were measured in both sites with vegetation and without vegetation and that were collected hourly, for 12 hours, and monthly, for four months. The file soilrespiration_data.csv contains these data, and the metadata file (soilrespiration_chammetadata.csv) and location metadata file (soilrespiration_locationmetadata.csv) have information on locations where the chambers were placed and sampled in the wetland. Data processing was done on raw methane fluxes (Flux_CH4) to remove the influence of ebullition (Flux_CH4_ebullition) to get a diffusive flux (Flux_CH4_diffusive).

54 ENVIRONMENTAL SCIENCES↗

The NASA Ames Research Center one- and two-dimensional stratospheric models. Part 1: The one-dimensional model

A one-dimensional model of stratospheric trace constituents is described in detail. Specifically, the numerical solution of the species continuity equations, including a technique for treating the stiff differential equations representing the chemical kinetic terms, and an appropriate method for simulating the diurnal variations of the species concentrations, are discussed. A specialized treatment of atmospheric photodissociation rates is outlined in the text. The choice of a vertical eddy diffusivity profile and its success in predicting the vertical tracer distributions (carbon 14, methane, and nitrous oxide) are also discussed.

Turco, R. P.↗

Diffusion Flame Stabilization

Diffusion flames are commonly used for industrial burners in furnaces and flares. Oxygen/fuel burners are usually diffusion burners, primarily for safety reasons, to prevent flashback and explosion in a potentially dangerous system. Furthermore, in most fires, condensed materials pyrolyze, vaporize, and burn in air as diffusion flames. As a result of the interaction of a diffusion flame with burner or condensed-fuel surfaces, a quenched space is formed, thus leaving a diffusion flame edge, which plays an important role in flame holding in combustion systems and fire spread through condensed fuels. Despite a long history of jet diffusion flame studies, lifting/blowoff mechanisms have not yet been fully understood, compared to those of premixed flames. In this study, the structure and stability of diffusion flames of gaseous hydrocarbon fuels in coflowing air at normal earth gravity have been investigated experimentally and computationally. Measurements of the critical mean jet velocity (U(sub jc)) of methane, ethane, or propane at lifting or blowoff were made as a function of the coflowing air velocity (U(sub a)) using a tube burner (i.d.: 2.87 mm). By using a computational fluid dynamics code with 33 species and 112 elementary reaction steps, the internal chemical-kinetic structures of the stabilizing region of methane and propane flames were investigated. A peak reactivity spot, i.e., reaction kernel, is formed in the flame stabilizing region due to back-diffusion of heat and radical species against an oxygen-rich incoming flow, thus holding the trailing diffusion flame. The simulated flame base moved downstream under flow conditions close to the measured stability limit.

Takahashi, Fumiaki↗

Rising methane emissions from boreal lakes due to increasing ice-free days

Lakes account for about 10% of the boreal landscape and are responsible for approximately 30% of biogenic methane emissions that have been found to increase under changing climate. However, the quantification of this climate-sensitive methane source is fraught with large uncertainty under warming climate conditions. Only a few studies have addressed the mechanism of climate impact on the increase of northern lake methane emissions. This study uses a large observational dataset of lake methane concentrations in Finland to constrain methane emissions with an extant process-based lake biogeochemical model. We found that the total current diffusive emission from Finnish lakes is 0.12±0.03 Tg CH4 yr-1 and will increase by 26-59% by the end of this century depending on different warming scenarios. We discover that while warming lake water and sediment temperature plays an important role, the climate impact on ice-on periods is a key indicator of future emissions. We conclude that these boreal lakes remain a significant methane source under the warming climate within this century.

54 ENVIRONMENTAL SCIENCES↗

Physical Properties and Gas Hydrate at a Near-Seafloor Thrust Fault, Hikurangi Margin, New Zealand

The Papaku Fault Zone, drilled at International Ocean Discovery Program (IODP) Site U1518, is an active splay fault in the frontal accretionary wedge of the Hikurangi Margin. In logging-while-drilling data, the 33-m-thick fault zone exhibits mixed modes of deformation associated with a trend of downward decreasing density, P-wave velocity, and resistivity. Methane hydrate is observed from ~30 to 585 m below seafloor (mbsf), including within and surrounding the fault zone. Hydrate accumulations are vertically discontinuous and occur throughout the entire logged section at low to moderate saturation in silty and sandy centimeter-thick layers. In this paper, we argue that the hydrate distribution implies that the methane is not sourced from fluid flow along the fault but instead by local diffusion. This, combined with geophysical observations and geochemical measurements from Site U1518, suggests that the fault is not a focused migration pathway for deeply sourced fluids and that the near-seafloor Papaku Fault Zone has little to no active fluid flow.

58 GEOSCIENCES↗

Diffusion Flame Stabilization

Diffusion flames are commonly used for industrial burners in furnaces and flares. Oxygen/fuel burners are usually diffusion burners, primarily for safety reasons, to prevent flashback and explosion in a potentially dangerous system. Furthermore, in most fires, condensed materials pyrolyze, vaporize, and burn in air as diffusion flames. As a result of the interaction of a diffusion flame with burner or condensed-fuel surfaces, a quenched space is formed, thus leaving a diffusion flame edge, which plays an important role in flame holding in combustion systems and fire spread through condensed fuels. Despite a long history of jet diffusion flame studies, lifting/blowoff mechanisms have not yet been fully understood, compared to those of premixed flames. In this study, the structure and stability of diffusion flames of gaseous hydrocarbon fuels in coflowing air at normal earth gravity have been investigated experimentally and computationally. Measurements of the critical mean jet velocity (U(sub jc)) of methane, ethane, or propane at lifting or blowoff were made as a function of the coflowing air velocity (U(sub a)) using a tube burner (i.d.: 2.87 mm) (Fig. 1, left). By using a computational fluid dynamics code with 33 species and 112 elementary reaction steps, the internal chemical-kinetic structures of the stabilizing region of methane and propane flames were investigated (Fig. 1, right). A peak reactivity spot, i.e., reaction kernel, is formed in the flame stabilizing region due to back-diffusion of heat and radical species against an oxygen-rich incoming flow, thus holding the trailing diffusion flame. The simulated flame base moved downstream under flow conditions close to the measured stability limit.

Takahashi, Fumiaki↗

Carbon flux measurements from chambers collected between April to October 2023 at Old Woman Creek, Huron, Ohio

This dataset contains carbon dioxide and methane gas flux measurements collected via chamber sampling at Old Woman Creek National Estuarine Research Reserve in Huron, OH. These data were generated to understand temporal and vegetation patterns associated with wetland carbon cycling. Specifically, this dataset intends to answer how carbon dioxide and methane fluxes change monthly and hourly across sites with vegetation and without vegetation. Data includes chamber measurements that were measured in both sites with vegetation and without vegetation and that were collected hourly (7 AM to 7 PM or 5 AM to 10 PM and monthly (April to October). The file soilrespiration_data23.csv contains these data, and the metadata file (soilrespiration_chammetadata23.csv) and location metadata file (soilrespiration_locationmetadata23.csv) have information on locations where the chambers were placed and sampled in the wetland. Data processing was done on raw methane fluxes (Flux_CH4) to remove the influence of ebullition (Flux_CH4_ebullition) to get a diffusive flux (Flux_CH4_diffusive).

54 ENVIRONMENTAL SCIENCES↗

2D imaging of absolute methyl concentrations in nanosecond pulsed plasma by photo-fragmentation laser-induced fluorescence

The methyl radical plays a central role in plasma-assisted hydrocarbon chemistry but is challenging to detect due to its high reactivity and strongly pre-dissociative electronically excited states. In this work, we report the development of a photo-fragmentation laser-induced fluorescence (PF-LIF) diagnostic for quantitative 2D imaging of methyl profiles in a plasma. This technique provides temporally and spatially resolved measurements of local methyl distributions, including in near-surface regions that are important for plasma-surface interactions such as plasma-assisted catalysis. The technique relies on photo-dissociation of methyl by the fifth harmonic of a Nd:YAG laser at 212.8 nm to produce CH fragments. These photofragments are then detected with LIF imaging by exciting a transition in the B-X(0, 0) band of CH with a second laser at 390 nm. Fluorescence from the overlapping A-X(0, 0), A-X(1, 1), and B-X(0, 1) bands of CH is detected near 430 nm with the A-state populated by collisional B-A electronic energy transfer. This non-resonant detection scheme enables interrogation close to a surface. The PF-LIF diagnostic is calibrated by producing a known amount of methyl through photo-dissociation of acetone vapor in a calibration gas mixture. We demonstrate PF-LIF imaging of methyl production in methane-containing nanosecond pulsed plasmas impinging on dielectric surfaces. Absolute calibration of the diagnostic is demonstrated in a diffuse, plane-to-plane discharge. Measured profiles show a relatively uniform distribution of up to 30 ppm of methyl. Relative methyl measurements in a filamentary plane-to-plane discharge and a plasma jet reveal highly localized intense production of methyl. The utility of the PF-LIF technique is further demonstrated by combining methyl measurements with formaldehyde LIF imaging to capture spatiotemporal correlations between methyl and formaldehyde, which is an important intermediate species in plasma-assisted oxidative coupling of methane.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Direct numerical simulation of single-species and binary-species boundary layers at high pressure

Direct numerical simulations of single-species and binary-species temporal boundary layers at high pressure are performed. The main objective is to investigate flow physics in a binary-species boundary layer at high pressure, with special attention to mass diffusion. The working fluids are nitrogen in the single-species cases, and a mixture of nitrogen and methane in the binary-species cases. An investigation of mean profiles shows that velocity and temperature profiles have steep gradients near the wall, whereas the mass fraction profiles do not have a steep gradient. This result indicates that the similarity law between velocity, temperature and mass fraction does not hold true in the binary-species boundary layer. The comparison of turbulent fluctuations shows that the qualitative characteristics of velocity and temperature are similar to each other. In contrast, profiles of mass fraction fluctuations are largely different from those of velocity and temperature. This result indicates that mass diffusion is not similar to momentum and thermal diffusions in binary-species boundary layers.

Toki, Takahiko↗

A Role of the Reaction Kernel in Propagation and Stabilization of Edge Diffusion Flames of C1-C3 Hydrocarbons

Diffusion flame stabilization is of essential importance in both Earth-bound combustion systems and spacecraft fire safety. Local extinction, re-ignition, and propagation processes may occur as a result of interactions between the flame zone and vortices or fire-extinguishing agents. By using a computational fluid dynamics code with a detailed chemistry model for methane combustion, the authors have revealed the chemical kinetic structure of the stabilizing region of both jet and flat-plate diffusion flames, predicted the flame stability limit, and proposed diffusion flame attachment and detachment mechanisms in normal and microgravity. Because of the unique geometry of the edge of diffusion flames, radical back-diffusion against the oxygen-rich entrainment dramatically enhanced chain reactions, thus forming a peak reactivity spot, i.e., reaction kernel, responsible for flame holding. The new results have been obtained for the edge diffusion flame propagation and attached flame structure using various C1-C3 hydrocarbons.

Takahashi, Fumiaki↗

Effect of gravity on methane-air combustion

Analytical and numerical techniques dealing with the theoretical description of the influence of zero and reduced gravitational acceleration on diffusion flames, with a view to improving understanding of fires in space vehicles, were developed in support of experimental work performed in this area. This was done in order to confirm qualitative understanding of the process, to determine the quantitative accuracy of numerical predictions, and to establish a mathematical model of the process for subsequent use as a predictive and exploratory tool. The following results were accomplished: (1) derivation of differential equations and boundary conditions describing the system, (2) details of the computations, using a FORTRAN computer program, for calculating the flow and heat and mass transfer in two dimensions (both steady and unsteady). It was shown that the experimental behavior can be reproduced with fair accuracy, provided that the time step is sufficiently short.

Elghobashi, S.↗