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At least 973 records · Page 54

Conversion of food waste to renewable energy: A techno-economic and environmental assessment

Increasing quantities of food waste have become a concern due to high disposal costs in landfills and high greenhouse gas emissions. With this increase in food waste generation, there is also an increasing demand for renewable natural gas to supplement traditional fossil fuel combustion and offset the impacts of climate change. Collecting food waste from landfills and turning it into renewable natural gas using anaerobic digestion could be a win-win option for both food waste disposal and renewable energy production. While some literature exists on the energy potential, economic feasibility, and environmental benefit of food waste disposal via anaerobic digestion, no existing study simultaneously evaluates the energy, economic and environmental effect of food waste to renewable energy via anaerobic digestion, especially on a plant and city scale. Further, this study is focused on the techno-economic and environmental assessment of food waste to energy via anaerobic digestion in order to fill this gap. Four anaerobic digestion pathways are considered in this study: flare, pipeline natural gas, combined heat and power, and combined cycle for efficient power generation. Using a city of 1M people the results show that renewable natural gas from food waste could supply the natural gas usage for 1.9% of residential use, 2.7% of commercial use, 1.1% of industrial use, 167.5% of the compressed natural gas vehicle fleet, 0.7% of electric power generation, or 2.5% of industrial high-temperature heating processes. All pathways except pipeline natural gas will have a positive net present value in the baseline scenario, and the pipeline natural gas pathway will become economically viable with a net present value of 31 USD/t of food waste with renewable energy credits. Lastly, all of the pathways achieve negative greenhouse gas emissions, which indicates that anaerobic digestion is a more environmentally friendly method for the handling of food waste than landfills.

03 NATURAL GAS↗

Some Notes on Neutron Up-Scattering and the Doppler-Broadening of High-Z Scattering Resonances

When neutrons are scattered by target nuclei at elevated temperatures, it is entirely possible that the neutron will actually gain energy (i.e., up-scatter) from the interaction. This phenomenon is in addition to the more usual case of the neutron losing energy (i.e., down-scatter). Furthermore, the motion of the target nuclei can also cause extended neutron down-scattering, i.e., the neutrons can and do scatter to energies lower than predicted by the simple asymptotic models. In recent years, more attention has been given to temperature-dependent scattering cross sections for materials in neutron multiplying systems. This has led to the inclusion of neutron up-scatter in deterministic codes like Partisn and to free gas scattering models for material temperature effects in Monte Carlo codes like MCNP and cross section processing codes like NJOY. The free gas scattering models have the effect of Doppler Broadening the scattering cross section output spectra in energy and angle. The current state of Doppler-Broadening numerical techniques used at Los Alamos for scattering resonances will be reviewed, and suggestions will be made for further developments. The focus will be on the free gas scattering models currently in use and the development of new models to include high-Z resonance scattering effects. These models change the neutron up-scattering behavior.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Development of Alternative Vacuum Pumps for Tritium Service

In tritium process systems, vacuum pumps are typically used to evacuate volumes and piping, as well as transfer gas to other parts of the process. This was done using the combination of an all-metal scroll pump with a metal bellows backing pump. The all-metal scroll pump, manufactured by Normetex, has been unavailable since 2012, and efforts continue to find a suitable replacement. The main obstacle is finding a pump that has no oils or polymer components, which degrade when exposed to tritium and introduce corrosive and/or hazardous impurities into the process. Since turbomolecular pumps are used in tritium processing, it is thought that pumps similar to the turbomolecular pumps would be of interest. The pumps would need to operate at lower rotational speeds to handle higher pressures and flow rates, which is best suited for Molecular Drag Pumps (MDP). To determine this, the vacuum pump characteristics must be determined for the MDP. This report details pump characteristics using an MDP backed by a Metal Bellows (Met-Bel) pump under static and flow conditions for various gases.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

SR19036 Improve TRP Cutter Head Performance

The Target Rod Preparation (TRP) cutter head motor suffers from overheating problems during Tritium Producing Burnable Absorber Rods (TPBAR) breaching operations. The TRP cell cutter head drive motor must remain below the administrative limit of 100°C during breaching operations. If temperatures in excess of 100°C are reached, work must be stopped, and the motor allowed to cool. The work stoppage due to overheating of the drive motor directly and drastically lowers the efficiency of the TPBAR breaching process, reducing the production of Tritium gas. Due to the increased need for Tritium gas, the overheating problem must be addressed to improve the overall efficiency of the TPBAR breaching process.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Alternative All-Metal Scroll Pump Design

In tritium process systems, vacuum pumps are typically used to evacuate volumes and piping, as well as transfer gas to other parts of the process. This was done using the combination of an all-metal scroll pump with a metal bellows backing pump. The all-metal scroll pump, manufactured by Normetex, has been unavailable since 2012, and efforts continue to find a suitable replacement. The main obstacle is finding a pump that has no oils or polymer components, which degrade when exposed to tritium and introduce corrosive and/or hazardous impurities into the process. There have been development efforts to design an all-metal scroll pump design alternative to the Normetex style. The first generation was fabricated out of machined stainless steel, but the thermal management and increased weight were not ideal. To mitigate the weight, an aluminum version was designed. The tritium holdup on untreated aluminum surfaces can be greater than stainless steel, so the wetted aluminum surfaces were electroless plated in nickel and then electroplated in gold. The development effort outlined in this report details the design of an improved version of the stainless steel version.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Engineering Scale Drying of Aluminum-Clad Spent Nuclear Fuel: Experiment Report

Engineering-scale tests were performed to evaluate the relative effectiveness of forced gas and vacuum-drying processes on aluminum-clad spent nuclear fuel (ASNF) in preparation for extended dry storage. Drying models were developed to improve confidence in the likely range of conditions at the start of dry storage and to understand the factors most significant to each process. Testing was performed at the Holtec International Forced Helium Dehydration training facility in Camden, New Jersey, by students from the University of South Carolina in collaboration with Idaho National Laboratory. A full-size Type 1a basket, with a full-diameter vessel configuration (based on the Department of Energy standardized canister design), was used in combination with a 10 assembly surrogate ASNF arrangement to provide a proxy for geometry. A resistance heater incorporated in one assembly simulated the influence of 100 W decay heat. This instrumented chamber allowed testing of the removal of bulk water, physisorbed water, and chemisorbed water over a range of operating parameters with either drying process. Thick oxide films were grown on aluminum test plates to mimic the ASNF surface chemistry. These one-use test plates were housed within select assemblies during drying. Post-test analysis of these plates gave a measure of the moisture removed during each test, which was compared to a control. Instrumentation provided detailed thermal, humidity, and gas or pressure data relevant to each test. Model simulations generally compared favorably to instrument data for the tests. While both processes were able to remove bulk water, removal of chemisorbed water was shown to depend heavily on local temperature. To the disadvantage of vacuum drying, operations approaching or exceeding 220°C achieved consistently more dehydroxylation.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Reduction of Iron‐Ore Pellets Using Different Gas Mixtures and Temperatures

Direct reduction of iron ore (DRI) is gaining an increased attention due to the growing need to decarbonize industrial processes. The current industrial DRI processes are performed using reformed natural gas, which results in CO 2 emission, although it is less than carbothermic reduction in the blast furnace. Carbon‐free reduction may be realized through the utilization of green H 2 as a reducing agent, in place of natural gas. Herein, the effects of various gas mixtures and temperature on the reduction kinetics of the hematite iron‐ore pellets are focused on in this work. Pellets are reduced at 700, 800, 850, and 900 °C in hydrogen and using various gas mixes at 850 °C. Morphology of the pellets is investigated with the help of scanning electron microscopy and mercury intrusion porosimetry. The effects of temperature and gas composition on the reduction kinetics and porosity of the pellets are discussed. A notable effect of reduction rate on the internal structure of the pellets is detected, slower reduction rate yielded bigger pores offsetting the gas composition. Higher temperature results in coarser pores and higher porosity. Finally, increase of CO content in the gas mix also leads to bigger pore size.

36 MATERIALS SCIENCE↗

Direct Study of Changes in Catalyst Structure-Kinetic Properties During Redox Transitions

The Temporal Analysis of Products (TAP) pulse response methodology is a transient technique that provides the time resolution needed to deconvolve reaction steps from the complex networks typical in industrial catalytic processes. Traditionally, TAP measurements observe gas phase dynamics at the reactor exit but lack direct measurements of changes in the catalyst itself. Recently, a new operando technique was developed that couples gas phase transients to dynamic changes in metal centers with the precise TAP methodology for nanomole titration. Using an industrial CrOx/Al2O3 catalyst used for propane dehydrogenation, we demonstrate the capabilities of this unique device to reveal key catalytic processes: 1) total propane oxidation not associated with chromia centers, 2) reduction of Cr6+ to Cr3+ correlated with selective product formation, and 3) subsequent carbon accumulation. By utilizing incremental pulsing in a diffusion-only transport regime, the spectrokinetic device allows us to resolve detailed changes in catalyst structure, composition, and kinetic function that are otherwise indistinguishable in conventional operando devices. The unification of the TAP methodology with time-resolved spectroscopic measurements offers new and unique insights into the complex kinetic phenomena regulated by solid catalyst surfaces.

03 - NATURAL GAS↗

On the Preconditioning of a Newton-Krylov Solver for a High-Order reconstructed Discontinuous Galerkin Discretization of All-Speed Compressible Flow with Phase Change for Application in Laser-Based Additive Manufacturing

This dissertation focuses on the development of a fully-implicit, high-order compressible ow solver with phase change. The work is motivated by laser-induced phase change applications, particularly by the need to develop large-scale multi-physics simulations of the selective laser melting (SLM) process in metal additive manufacturing (3D printing). Simulations of the SLM process require precise tracking of multi-material solid-liquid-gas interfaces, due to laser-induced melting/ solidi cation and evaporation/condensation of metal powder in an ambient gas. These rapid density variations and phase change processes tightly couple the governing equations, requiring a fully compressible framework to robustly capture the rapid density variations of the ambient gas and the melting/evaporation of the metal powder. For non-isothermal phase change, the velocity is gradually suppressed through the mushy region by a variable viscosity and Darcy source term model. The governing equations are discretized up to 4th-order accuracy with our reconstructed Discontinuous Galerkin spatial discretization scheme and up to 5th-order accuracy with L-stable fully implicit time discretization schemes (BDF2 and ESDIRK3-5). The resulting set of non-linear equations is solved using a robust Newton-Krylov method, with the Jacobian-free version of the GMRES solver for linear iterations. Due to the sti nes associated with the acoustic waves and thermal and viscous/material strength e ects, preconditioning the GMRES solver is essential. A robust and scalable approximate block factorization preconditioner was developed, which utilizes the velocity-pressure (vP) and velocity-temperature (vT) Schur complement systems. This multigrid block reduction preconditioning technique converges for high CFL/Fourier numbers and exhibits excellent parallel and algorithmic scalability on classic benchmark problems in uid dynamics (lid-driven cavity ow and natural convection heat transfer) as well as for laser-induced phase change problems in 2D and 3D.

42 ENGINEERING↗

Investigations of effect of phase change mass transfer rate on cavitation process with homogeneous relaxation model

The super high fuel injection pressure and micro size of nozzle orifice has been an important development trend for the fuel injection system. Accordingly, cavitation transient process, fuel compressibility, amount of noncondensable gas in the fuel and cavitation erosion have attracted more attention. Based on the fact of cavitation in itself is a kind of thermodynamic phase change process, this paper takes the perspective of the cavitation phase change mass transfer process to analyze above mentioned phenomenon. The two-phase cavitating turbulent flow simulations with VOF approach coupled with HRM cavitation model and U-RANS of standard k-ε turbulence model were performed for investigations of cavitation phase change mass transfer process. It is concluded the mass transfer time scale coefficient in the Homogenous Relaxation Model (HRM) representing mass transfer rate should tend to be as small as possible in a condition that ensured the solver stable. At very fast mass transfer rate, the phase change occurs at very thin interface between liquid and vapor phase and condensation occurs more focused and then will contribute predictably to a more serious cavitation erosion. Both the initial non-condensable gas in fuel and the fuel compressibility can accelerate the cavitation mass transfer process.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

A global anthropogenic emission inventory of atmospheric pollutants from sector- and fuel-specific sources (1970–2017): an application of the Community Emissions Data System (CEDS)

Global anthropogenic emission inventories remain vital for understanding the sources of atmospheric pollution and the associated impacts on the environment, human health, and society. Rapid changes in today's society require that these inventories provide contemporary estimates of multiple atmospheric pollutants with both source sector and fuel type information to understand and effectively mitigate future impacts. To fill this need, we have updated the open-source Community Emissions Data System (CEDS) (Hoesly et al., 2019) to develop a new global emission inventory, CEDSGBD-MAPS. This inventory includes emissions of seven key atmospheric pollutants (NOx; CO; SO2; NH3; non-methane volatile organic compounds, NMVOCs; black carbon, BC; organic carbon, OC) over the time period from 1970–2017 and reports annual country-total emissions as a function of 11 anthropogenic sectors (agriculture; energy generation; industrial processes; on-road and non-road transportation; separate residential, commercial, and other sectors (RCO); waste; solvent use; and international shipping) and four fuel categories (total coal, solid biofuel, the sum of liquid-fuel and natural-gas combustion, and remaining process-level emissions). The CEDSGBD-MAPS inventory additionally includes monthly global gridded (0.5°?×?0.5°) emission fluxes for each compound, sector, and fuel type to facilitate their use in earth system models. CEDSGBD-MAPS utilizes updated activity data, updates to the core CEDS default scaling procedure, and modifications to the final procedures for emissions gridding and aggregation. Relative to the previous CEDS inventory (Hoesly et al., 2018), these updates extend the emission estimates from 2014 to 2017 and improve the overall agreement between CEDS and two widely used global bottom-up emission inventories. The CEDSGBD-MAPS inventory provides the most contemporary global emission estimates to date for these key atmospheric pollutants and is the first to provide global estimates for these species as a function of multiple fuel types and source sectors. Dominant sources of global NOx and SO2 emissions in 2017 include the combustion of oil, gas, and coal in the energy and industry sectors as well as on-road transportation and international shipping for NOx. Dominant sources of global CO emissions in 2017 include on-road transportation and residential biofuel combustion. Dominant global sources of carbonaceous aerosol in 2017 include residential biofuel combustion, on-road transportation (BC only), and emissions from the waste sector. Global emissions of NOx, SO2, CO, BC, and OC all peak in 2012 or earlier, with more recent emission reductions driven by large changes in emissions from China, North America, and Europe. In contrast, global emissions of NH3 and NMVOCs continuously increase between 1970 and 2017, with agriculture as a major source of global NH3 emissions and solvent use, energy, residential, and the on-road transport sectors as major sources of global NMVOCs. Due to similar development methods and underlying datasets, the CEDSGBD-MAPS emissions are expected to have consistent sources of uncertainty as other bottom-up inventories. The CEDSGBD-MAPS source code is publicly available online through GitHub: https://github.com/emcduffie/CEDS/tree/CEDS_GBD-MAPS (last access: 1 December 2020). The CEDSGBD-MAPS emission inventory dataset (both annual country-total and monthly global gridded files) is publicly available under https://doi.org/10.5281/zenodo.3754964 (McDuffie et al., 2020c).

Mcduffie, Erin↗

NiAl Oxidation Reaction Processes Studied In Situ Using MEMS-Based Closed-Cell Gas Reaction Transmission Electron Microscopy

The nanoscale oxidation mechanisms and kinetics of a model β-NiAl system were investigated using in situ closed-cell gas reaction scanning transmission electron microscopy (STEM). Here, we directly visualize the dynamic structural and chemical changes that occur during high-temperature oxidation at a high spatial resolution of 50.3Ni–49.7Al (at.%) nanoparticles under static air conditions at 730 Torr with heating up to 750 °C at 5 °C/s. A MEMS-based gas cell system, with microfabricated heater devices and a gas delivery system, was used to reveal site-specific oxidation initiation sites. Through time-resolved annular dark-field STEM imaging, we tracked the nanoscale oxidation kinetics of Al 2 O 3 . After oxidation at 750 °C, nucleation of voids at the Ni/Al 2 O 3 interface was observed along a NiAl grain boundary, followed by the formation of faceted NiO crystals. Small faceted cubic crystals of NiO were formed at the initial stage of oxidation at high PO 2 due to the outward self-diffusion of Ni 2+ ions, followed by the formation of a mixture of metastable and stable α-Al 2 O 3 at the oxide/metal interface that is attributed to a PO 2 decrease with oxidation time, which agreed with thermodynamic modeling calculations. Furthermore, the results from these in situ oxidation experiments in the β-NiAl system are in agreement with the established oxidation mechanisms; however, with in situ closed-cell gas microscopy it is now feasible to investigate nanoscale oxidation mechanisms and kinetics in real time and at high spatial resolution and can be broadly applied to understand the basic high-temperature oxidation mechanisms for a wide range of alloy compositions.

36 MATERIALS SCIENCE↗

Ecton processes in the generation of pulsed runaway electron beams in a gas discharge

As was shown earlier for pulsed discharges that occur in electric fields rising with extremely high rates (10{sup 18} V/(cm s)) during the pulse rise time, the electron current in a vacuum discharge is lower than the current of runaway electrons in an atmospheric air discharge in a 1-cm-long gap. In this paper, this is explained by that the field emission current from cathode microprotrusions in a gas discharge is enhanced due to gas ionization. This hastens the initiation of explosive electron emission, which occurs within 10{sup –11} s at a current density of up to 10{sup 10} A/cm{sup 2}. Thereafter, a first-type cathode spot starts forming. The temperature of the cathode spot decreases due to heat conduction, and the explosive emission current ceases. Thus, the runaway electron current pulse is similar in nature to the ecton phenomenon in a vacuum discharge.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Effect of Recrystallization on Gas Bubble Swelling in UMo Fuels

The development of low-enriched uranium (LEU) fuels such as UMo dispersion fuels and monolithic UMo fuels is part of a global effort on nuclear nonproliferation. Although UMo fuels have the advantage of high density, excellent irradiation performance and good thermal conductivity, the volumetric swelling in irradiated metallic fuels is known to be an important design parameter because it affects not only the thermal conductivity of the fuels but also the mechanical integrity of fuel structures. Experiments also show that recrystallization dramatically affects the gas bubble swelling kinetics. A series of materials processes such as casting, mechanical rolling and thermal treatment are used in fuel fabrication. Resulting microstructure, such as grain size, porosity, and second phase, strongly depends on the material processes and process parameters. Therefore, a fundamental understanding how fabricated microstructures and irradiation conditions affect the nucleation of gas bubbles, recrystallization and gas bubble swelling kinetics is essential for optimizing material processes to obtain desired microstructure and fuel performance. Great effort has been made in the development of modeling capability for predicting gas bubble swelling kinetics and fission gas release kinetics in nuclear fuels. However, these models are based on the assumptions that the inter- and intra-granular gas bubble sizes are independent of position and only depend on time or fission density. Therefore, they are applicable to a material with uniform microstructure such as equiaxed grains with homogeneous defect distributions, homogeneous thermodynamic and kinetic properties of defects, and uniform radiation conditions. Very recently, we developed a three dimension (3D) microstructure dependent gas bubble swelling model for investigating the effect of heterogeneous microstructures and inhomogeneous thermodynamic properties of defects on gas bubble swelling in polycrystalline UMo fuels. However, the model doesn't take into account the effect of recrystallization on swelling kinetics. In this work, the spatially dependent rate theory is used to describe the evolution of interstitials and interstitial loop density. Recrystallization is described by a phase-field model with a concept of 'phase transition' when the local interstitial loop density is larger than a critical value. The intra- and inter- granular gas bubble evolution is described by the spatially dependent Booth model. A model integrating all the microstructure evolution enables one to study the effect of heterogeneous microstructures, recrystallization, and the metallic fuel thermodynamic and kinetic properties on gas bubble swelling kinetics.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Non-Equilibrium in a Dust-Forming Low-Temperature Plasma: A CARS Study

Dust-forming low-temperature plasmas are versatile systems for the production of nanoparticles with tunable functionalities. While attractive from a materials processing point of view, these systems are inherently complex, with several plasma-induced phenomena determining the properties of the produced materials. Here, we characterize a carbon nanoparticle-forming plasma using coherent anti-Stokes Raman spectroscopy (CARS), with the primary goal of measuring gas temperature. While gas temperature is typically assumed to be at or slightly above room temperature in these reactors, we measure gas temperatures exceeding 1000 K under typical process conditions. We find a correlation between the gas temperature and the nanoparticle yield, suggesting that the particle nucleation and growth process releases energy within the reaction volume, leading to significant gas heating. In addition, we find that the relaxation of vibrationally excited species at the particle surfaces is a major contributor to their heating. In conclusion, these results underscore the complexity of these systems and the need for their more in-depth characterization using advanced techniques such as CARS.

Basic Plasma Phenomena and Gas Discharges↗

Life Extension of Nuclear Plant Facilities through Monitoring and Detailed Analysis - 16175

The UK has accumulated a substantial legacy of radioactive waste from various civil nuclear and defence programmes. Presently, however most of the UK radioactive waste is generated from nine power stations which generate approximately one sixth of the of the country's electricity. Irradiated fuel is removed from these reactors and safe management of the radioactive solid and liquid effluents is required. The safe management of these effluents is essential. Sellafield, in West Cumbria UK, contains two reprocessing plants, one designed to process nuclear fuel from Magnox reactors (CO{sub 2} cooled with Uranium bar fuel) and the other to process nuclear fuel from Advanced Gas cooled Reactors and Pressurized Water Reactors. The reprocessing stage enables extraction of fissile material for recycling. This leaves a volume of dilute but high-level waste. The high-level radioactive liquid waste is concentrated to reduce its volume and then incorporated into borosilicate glass, using a process called vitrification. The glass is then poured into stainless steel containers and placed in long term storage. This required concentration of HLW liquor is achieved using a suite of aging evaporators. All evaporators are of similar design constructed from corrosion resistant stainless steel having dimensions height ∼11 m, internal diameter 3.05 m and capable of holding 13.7 m{sup 3} of liquor. The basic principle of operation is to heat the dilute liquor under partial vacuum, at constant volume, until the target concentration is achieved. Heating of the liquor is achieved using steam heated coils within the evaporator, and steam in the jacket which surrounds the lower half of the evaporator vessel. The evaporator is then brought to atmospheric pressure and the concentrated liquor is ejected whilst hot. The evaporator is then cooled with water cooled coils and a water filled jacket. New dilute liquor is then added for a new batch. The process is then repeated. As the evaporators reach the end of their original design life accurate prediction of the current condition of nuclear plant facilities is essential to safely justify continued plant operation by ensuring structural integrity. This poses a significant challenge as many aging UK nuclear facilities were not inherently built with inspection in mind. The potential life limiting components of the HA evaporators at Sellafield are the surfaces that contact the product liquor at elevated temperatures i.e. the steam heated surfaces of the coils within the evaporator vessel and the vessel base and wall surrounded by the steam jacket. Each heating component is critical to the operational life of the evaporator - the removal from service of a coil heating component significantly reduces the operational flexibility and remnant life of this plant. Over the last decade a variety of cutting-edge expertise and methodologies have been utilised to accurately measure and then predict the current condition of the plant and also to predict its remnant life. This paper provides an overview of the development of several techniques deployed, namely non-destructive testing/inspection, in-house software development and finite element modelling. These methods have been validated by lab-scale or full-scale experiments along with historical plant data. These techniques have been evolved and refined for over a decade, providing vital insights into the physical behaviour of this complex reprocessing system. This enables not only accurate assessment of the current condition of the plant equipment but also allows scientifically underpinned predictions to be made of how it will behave into the future. This is critical for Sellafield as this knowledge feeds into their safety case to the Office of Nuclear Regulation to justify continued operation. It is concluded that this integrated approach provides a robust analysis tool which has driven change and optimisation of plant procedures ensuring continued safe operation whilst extending the life of the facility. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Linking pore-scale and basin-scale effects on diffusive methane transport in hydrate bearing environments through multi-scale reservoir simulations

We explore the gas hydrate-generating capacity of diffusive methane transport induced by solubility gradients due to pore size contrasts in lithologically heterogeneous marine sediments. Through the use of 1D, 2D, and 3D reactive transport simulations, we investigate scale-dependent processes in diffusion-dominated gas hydrate systems. These simulations all track a sand body, or series of sands, surrounded by clays as they are buried through the gas hydrate stability zone. Methane is sourced by microbial methanogenesis in the clays surrounding the sand layers. In 1D, simulations performed in a Lagrangian reference frame demonstrate that gas hydrate in thin sands (3.6 m thick) can occur in high saturations (upward of 70%) at the edges of sand bodies within the upper 400 meters below the seafloor. Diffusion of methane toward the center of the sand layer depends on the concentration gradient within the sand: broader sand pore size distributions with smaller median pore sizes enhance diffusive action toward the sand’s center. Incorporating downhole log- and laboratory-derived sand pore size distributions, gas hydrate saturations in the center of the sand can reach 20% of the hydrate saturations at the sand’s edges. Furthermore, we show that hydrate-free zones exist immediately above and below the sand and are approximately 5 m thick, depending on the sand-clay solubility contrast. A moving reference frame is also adopted in 2D, and the angle of gravity is rotated relative to the grid system to simulate a dipping sand layer. This is important to minimize diffusive edge effects or numerical diffusion that might be associated with a dipping sand in an Eulerian grid system oriented orthogonal to gravity. Two-dimensional simulations demonstrate the tendency for gas hydrate to accumulate downdip in a sand body because of greater methane transport at depth due to larger sand-clay solubility contrasts. In 3D, basin-scale simulations illuminate how convergent sand layers in a multilayered system can compete for diffusion from clays between them, resulting in relatively low hydrate saturations. All simulations suggest that when hydrate present in clays dissociates with burial, the additional dissolved methane is soaked up by nearby sands preserving high hydrate saturations.

Nole, Michael↗