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At least 451 records · Page 25

Electrochemical conversion of methane to ethylene, olefins, and paraffins using metal-supported solid oxide cells

Electrochemical oxidative coupling of methane (E-OCM) with Sr 2 Fe 1·5 Mo 0·5 O 6–δ (SFM) catalyst is demonstrated with metal-supported solid oxide cells (MS-SOC). SFM anode and Pr 6 O 11 cathode catalysts are loaded into a porous symmetric-architecture cell by infiltration and firing. The most effective chelating agent (citric acid/ethyl glycol) and optimal firing/reducing temperatures (850 °C/750 °C) for the SFM catalyst precursor solution are selected and confirmed by cell testing. Operating temperature, cell voltage, and oxygen concentration at the cathode greatly affect the methane conversion rate and product selectivity by controlling the oxygen ion flow. CH 4 conversion of 85.8% is obtained, with C 2 H 4 , C 2 H 6 , and H 2 concentrations of 10.5%, 12.3%, and 25.6% at 800 °C, respectively, in the product exhaust gas. Reasonable stability of the current density and methane conversion is demonstrated during 200 h operation. Furthermore, this research demonstrates technical progress in catalyst and device development for the E-OCM reaction to synthesize valuable chemicals.

30 DIRECT ENERGY CONVERSION↗

Reaction heterogeneity in practical high-energy lithium–sulfur pouch cells

The lithium–sulfur (Li–S) battery is a promising next-generation energy storage technology because of its high theoretical energy and low cost. Extensive research efforts have been made on new materials and advanced characterization techniques for mechanistic studies. However, it is uncertain how discoveries made on the material level apply to realistic batteries due to limited analysis and characterization of real high-energy cells, such as pouch cells. Evaluation of pouch cells (>1 A h) (instead of coin cells) that are scalable to practical cells provides a critical understanding of current limitations which enables the proposal of strategies and solutions for further performance improvement. Herein, we design and fabricate pouch cells over 300 W h kg -1 , compare the cell parameters required for high-energy pouch cells, and investigate the reaction processes and their correlation to cell cycling behavior and failure mechanisms. Spatially resolved characterization techniques and fluid-flow simulation reveal the impacts of the liquid electrolyte diffusion within the pouch cells. We found that catastrophic failure of high-energy Li–S pouch cells results from uneven sulfur/polysulfide reactions and electrolyte depletion for the first tens of cycles, rather than sulfur dissolution as commonly reported in the literature. The uneven reaction stems from limited electrolyte diffusion through the porous channels into the central part of thick cathodes during cycling, which is amplified both across the sulfur electrodes and within the same electrode plane. A combination of strategies is suggested to increase sulfur utilization, improve nanoarchitectures for electrolyte diffusion and reduce consumption of the electrolytes and additives.

25 ENERGY STORAGE↗

Lithium extraction composite for recovery of lithium from brines, and process of using said composition

A lithium extraction composite comprising: (i) a porous support and (ii) particles of a lithium-selective sorbent material coated on at least one surface of the support, wherein the support has a planar membrane, fiber (or rod), or tubular shape. A method for extracting and recovering a lithium salt from an aqueous solution by use of the above-described composition is also described, the method comprising (a) flowing the aqueous source solution through a first zone or over a first surface of the lithium extraction composite to result in selective lithium intercalation in the lithium-selective sorbent material in the first zone or first surface; and (b) simultaneously recovering lithium salt extracted in step (a) from said lithium-selective sorbent material by flowing an aqueous stripping solution through a second zone or over a second surface of the lithium extraction composite in which lithium ions from the first zone or first surface diffuse.

Bhave, Ramesh R.↗

Wash Penalty Factors: Insight into the Effects of Water Wash Down of Building Materials for Radionuclide/Nuclear (Rn) Decontamination - 20153

The release of radiological material to the urban environment can have a devastating socio-economic impact. In an urban release scenario, areas around the dispersal epicenter and any areas contaminated via atmospheric deposition may require extensive decontamination. Most recently, our group reported the decontamination efficacy of pressurized water washing of common porous building materials, and compared the penetration depth of the contaminations before and after exposure to pressurized tap water. Here, we continue evaluation of the decontamination efficacy of wash solutions based on potassium (K{sup +}) salt for cesium (Cs), strontium (Sr), and europium (Eu) contaminations on common building surfaces. The surfaces included: the cement used in concrete, the aggregate used in concrete, intact concrete, roadway asphalt, asphalt shingles, and latex paint. We deposited solutions of {sup 137}Cs, {sup 85}Sr, and {sup 152}Eu onto numerous common building materials and exposed these materials to a static bath or low-pressure flow of tap water, 0.1 M potassium chloride (KCl), and 0.5 M KCl. The decontamination efficacy and the depth profile for residual contamination were measured to determine the conditions under which applying a wash solution has benefit compared to physically removing the surface material. To aid in these analyses, we introduced a 'wash penalty factor' to quantify the degree to which contamination migrated into the bulk material by the action of the wash method. On asphalt, 70-80% of the radionuclides were found to be within 0.02 mm of the surface. Cs{sup +} bonded to negative charge sites on the surface of the mineral aggregate (used in concrete) so decontamination was improved by ion exchange with K{sup +}. Sr{sup 2+} is soluble and removed by water, while not bonding to aggregate or demonstrating solubility in the liquid asphalt. Eu{sup 3+} is precipitated and not removed in gentle wash but displays mobility within the pore space that suggests its presence as a colloid. Concrete is more porous than asphalt, and 80% of the radionuclides were within 0.2 mm of the surface for {sup 137}Cs and {sup 152}Eu and 50- 80% for {sup 85}Sr. On concrete, Cs{sup +} bonds similarly to asphalt. Sr{sup 2+} bonds to the cement or precipitates from the alkaline pore water. Eu{sup 3+} sorbs to the cement and then precipitates. In brick, the results for Cs{sup +} and Sr{sup 2+} suggested that diffusion of ions from deeper in the coupon was important. Eu{sup 3+} is removed poorly due to precipitation. We will explain and report example wash penalty factors that vary from 0 to > 1 for the various methods and the implications for deciding when to implement wash down methods. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Penetration of Fission Products Ions into Complex Solids and the Effect of Ionic Wash Methods

During washing of radiologically impacted building surfaces, penetration of radionuclide ions into complex solids associated with these surfaces may occur. This study investigates the penetration of Cs-137, Sr-85, and Eu-152 solutions into numerous common building materials and radionuclide behavior when these materials were exposed to a static bath or low-pressure flow of tap water, 0.1 M potassium chloride (KCl), and 0.5 M KCl. The decontamination efficacy and the depth profile for residual contamination were measured to determine the conditions under which applying a wash solution has benefit compared to physically removing the surface material. On asphalt, 70-80% of the radionuclides were found to be within 0.02 mm of the surface. Concrete is more porous than asphalt, and 80% of the radionuclides were within 0.2 mm of the surface for Cs-137 and Eu-152 and 50-80% for Sr-85. Water effectively removed all contaminants from hard nonporous surfaces. Finally, this paper illustrates that a wash penalty factor concept-defined as ratio of the depth at which 50% of the radioactivity is found in the washed sample divided by the depth at which 50% of radioactivity is found in the control-can serve as a way to quantify whether the wash method increases the depth at which contamination penetrates into the material and thus the material becomes more difficult to decontaminate.

building materials↗

Development and Validation of Resistance-Capacitance Model for Phase Change Material Embedded in Porous Media

A simple and effective way to enhance PCM thermal conductivity is by embedding porous materials with high thermal conductivities. In this work, CFD was used to evaluate the melting of PCM embedded in metal foam supplied with constant heat flux. Good agreement between experimental and numerical results has been found with a mean PCM local temperature deviation of 1.62K and 2.97K in two locations. The CFD simulation time was 56 hours for 6.5 hours of flow time. A computationally efficient resistance capacitance-based model (RCM) was developed to improve simulation speed. The proposed RCM exhibited mean local temperature deviations of 1.86K and 2.96K when compared against the experimental data for two thermocouple positions, however, it was approximately 2.5x10 5 times faster than CFD. The charging time deviation was less than 1% compared to CFD, and no significant change in thermal energy stored was observed since the temperature differences were small enough to result in insignificant sensible heat deviation. A simulation cost-effectiveness index (CEI) considering accuracy and computational affordability was introduced; the CEI of the RCM solver is 10 3 times better compared to CFD for the prediction of local PCM temperature.

25 ENERGY STORAGE↗

Water production for coffee brewing by electrodeionization

A resin-wafer electrodeionization (RW-EDI) apparatus for purifying water for coffee brewing comprises a cathode; an anode; and multiple porous solid resin wafer exchange units arranged in a stack between the cathode and the anode, and an air distributor adapted and arranged to aerate the water to be purified. Each unit comprises a monovalent cation exchange membrane (CEM), an anion exchange membrane (AEM), and an ion exchange resin wafer between the CEM and the AEM, which is in contact with, and in fluid flow connection with the CEM and AEM. Each resin wafer comprises a cation exchange resin and an anion exchange resin. The units are oriented with the CEM facing the cathode and the AEM facing the anode, with space between the units defining ion concentrate chambers. Bipolar ion exchange membranes separate the anode and cathode from their nearest resin wafer exchange units.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Methane foam performance evaluation in water-wet unconsolidated porous media: A systematic experimental investigation at elevated pressure and temperature conditions

In the petroleum industry, enhanced oil recovery (EOR) techniques employ foam extensively to establish conformance control in heterogeneous and fractured reservoirs in order to increase the sweep efficiency. In such applications, foam performance evaluation under complex subsurface conditions is pivotal for the effective and optimized deployment of foam treatment. However, there is a scarcity of hydrocarbon gas foam generation and evaluation studies that examine the relationships between foam performance and the critical foam parameters at high-pressure and high-temperature conditions. Here, this study aims at methodically investigating the effects of several foam parameters on methane foam performance in water-wet proppant packs under harsh operating conditions. This is in relation to the technical needs of hydrocarbon foam injection into hydraulically-induced, propped fractures in unconventional oil reservoirs. To this end, a state-of-the-art experimental foam generation apparatus was designed, fabricated, and commissioned. We performed a large number of foam flow experiments on proppant packs using methane gas and different foaming agents at 3500 psi and 115°C. Anionic and amphoteric surfactants were employed to probe the effect of their ionic nature on foam performance. Foam performance sensitivities to various foam generation parameters and operating conditions, such as surfactant concentration, gas fraction, total injection rate, operating pressure, salinity, and proppant pack length were investigated. To this end, steady-state pressure drops across the proppant packs during foam generation and foam's apparent viscosity were measured to quantify the foam performance of surfactants. The results were then analyzed to determine optimum values of the foam parameters and the interplay between these parameters are discussed here. The systematic results achieved from this work are in agreement with the trends available in the literature and provide new insights into complexities of in situ foam generation in water-wet, unconsolidated porous media at extreme reservoir conditions.

03 NATURAL GAS↗

SCM overview & the EBR-II shutdown heat removal tests validation.

Pronghorn is an engineering-scale, coarse-mesh, thermal-hydraulics tool for supporting reactor-core simulations of advanced nuclear reactors. Most of the current efforts in Pronghorn have been devoted in developing porous finite-volume capabilities and adapting closure correlations for coarse-mesh thermal-hydraulics modeling. However, for liquid-metal reactors (LMRs) with wire-wrapped fuel pin assemblies, a pin-level thermal-hydraulic resolution is required for most safety case studies (pin rupture, channel blockage, etc.). For this purpose, a new Subchannel application is developed in MOOSE, which affords the required flow field resolution, while still preserving an engineering-scale approach. This new solver can be natively coupled to Pronghorn and other MOOSE objects to enable full-core, multi-physics, multi-scale engineering studies. This presentation presents the main features of the SCM code and demonstrates a validation case based on the EBR-II SHRT tests.

21 - SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLAN↗

Interfacial engineering via laser ablation for high-performing PEM water electrolysis

A rationalized interfacial design strategy was applied to tailor the porous transport layer (PTL)-catalyst layer (CL) contact and the PTL bulk-phase architecture. Particularly, at the PTL-CL interface, our results reveal that laser ablated sintered titanium power-based PTLs improve electrolyzer performance at both the H2NEW Consortium baseline catalyst loading of 0.4 mgIr cm -2 as well as at the ultra-low catalyst loading of 0.055 mgIr cm -2 . Under ultra-low catalyst loadings, the laser ablated PTL demonstrates maximum reduction of 230 mV compared to the commercial PTL at 4 A cm -2 , and reduces by 68 mV at 3.2 A cm -2 under H2NEW baseline loading. Laser ablation alters the titanium phase at the interface, so it forms more uniform structure like a microporous layer or a backing layer, leading to an increase in the surface area in contact with the catalyst layer while preventing the membrane from deforming into the PTL. Moreover, we reveal that bulk-phase architecture modification of the PTL by ablating patterned pores at the flow field-PTL interface improves mass transport without sacrificing contact at the CL-PTL interface. Overall, laser ablation of the PTL is an effective method to customize interfacial design to enhance proton exchange membrane electrolyzer performance.

08 HYDROGEN↗

An integrated coupling model for solving multiscale fluid-fluid coupling problems in SAM code

In this study, an integrated coupling method has been developed for solving multiscale fluid-fluid coupling problems in plant-scale safety analysis models in SAM (System Analysis Module) code. In this method, a higher-fidelity multi-dimensional (3D) flow module is used for reactor components of complex flow features (e.g., reactor core) and a lumped parameter one-dimensional (1D) flow module for plant-scale flow loops (e.g., primary loop pipe network), respectively. In this method, the 3D fluid equation/domain and 1D fluid equation/domain are tightly coupled at the residual level and solved simultaneously using the Newton’s method to overcome the convergence issues typically seen in existing approaches like separate domain approach, where the 3D fluid equation and 1D fluid equation are solved separately. Extensive and successful code verifications and demonstrations have been performed for this newly developed method. This new modeling approach significantly simplify the work flow in developing high-fidelity plant-scale safety analysis model, e.g. for pool-type reactors and pebble-bed reactors.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Gas-Cooled High-Temperature Pebble-Bed Reactor Reference Plant Model

This report details a fully coupled neutronics thermal hydraulics reference plant model for a gas-cooled high-temperature pebble-bed reactor. The multiphysics model is developed on the Nuclear Regulatory Commission's Comprehensive Reactor Analysis Bundle (BlueCRAB) available on the Idaho National Laboratory high performance computer, which natively and seamlessly couples Griffin, Pronghorn, and the BISON MOOSE-based applications. Griffin provides the reactor physics capabilities including depletion to the equilibrium core, k-eigenvalue, adjoint, and transient solutions. Pronghorn solves the porous medium equations for the fluid regions and conduction in the solid regions. BISON solves thermal conduction problems for the average pebble and TRISO in the pebble-bed core thus providing the fuel and moderator spatial fields for each pebble burnup group. The neutronics feedback relies primarily on fuel and moderator temperatures. We present results for the coupled steady state equilibrium core and a protected loss of flow event. Although this model is to be considered prototypical with regard to the capabilities in BlueCRAB, its results are consistent with published work by the Institute of Nuclear and New Energy Technology (INET) in China and other research entities.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Impact of Porous Transport Layer In-Plane Conduction on Spatially Resolved Current and EIS Measurements in a Proton Exchange Membrane Water Electrolyzer

An XY segmented cell was developed for low temperature PEM water electrolysis (PEMWE). The system can assess the local performance by enabling in situ measurements of spatial currents and impedances. In this work, we show through experiments, as well as through modelling work, that the porous transport layer (PTL) must be segmented to eliminate crosstalk. Accurate measurements are only possible when crosstalk is fully eliminated. The XY segmented cell is applied to a case study characterizing the impact of a PTL platinum coating void on spatial performance. The localized performance impact of the coating void is found to be orientation specific: coating voids facing the catalyst layer reduce performance significantly more than coating voids facing the flow field. The results suggest that the tolerances for PTL coating uniformity can be lower at the side facing the flow field. The work showcases the feasibility of the XY segmented cell for impact assessment studies. The presented XY segmented cell enables the characterization of spatial phenomena in PEMWE devices and is envisioned to support modeling efforts and the investigation of manufacturing related tolerances for mass produced PEMWE devices.

08 HYDROGEN↗

Analysis of convection heat transfer on multiscale rough superhydrophobic and liquid infused surfaces

Multiscale rough superhydrophobic or slippery liquid infused porous surfaces have gained much interest in recent years for their improved transport phenomena properties. While there have been several studies on drag reduction and condensation on non-wetting surfaces, convection heat transfer that is important in many thermal and thermochemical applications has not been addressed systematically. Here, this article utilizes a fractal description of rough surface topographies to develop analytical models for the Nusselt number and the thermal hydraulic factor for fluid flow and heat transfer inside a cylinder with non-wetting surfaces. For air-infused superhydrophobic surfaces, the model considers the dynamic stability of the air/fluid interface in the asperities. Using the analytical formulations and the stability criteria, systematic studies are presented on the effects of the fractal surface parameters, cylinder radius and Reynolds number on the convective heat transfer characteristics, from which surface texture design maps are developed for maximizing the convection heat transfer. It is shown that multiscale non-wetting surfaces are most effective in the range of lower Reynolds number and small cylinder radius for achieving the best convective heat transfer and thermal hydraulic performance. Applying the models to actual non-wetting surface topographies fabricated using electrodeposition and chemical etching, it is shown that contrary to prevailing notion, superhydrophobicity, characterized by the highest contact angles, does not always lead to the maximum convective heat transfer performance, and that under certain fluid flow conditions, hydrophobic surfaces may offer a greater thermal performance.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Surface oxygenation induced strong interaction between Pd catalyst and functional support for zinc–air batteries

Employing the strong metal-support interaction (SMSI) effect for promoting the catalyst's activity toward the oxygen reduction reaction (ORR) is promising due to the electronic structure optimization and high utilization efficiency of platinum group metal (PGM) catalysts. Metal oxides as alternative supports for PGMs facilitate intrinsic activity and improve durability as compared to conventional carbon supports. However, the restricted mass and electron transfer at the metal/support interface need to be addressed. Herein, to strengthen the interaction at the metal/support interfaces and improve the utilization efficiency of PGM, an ultralow loading of Pd was embedded in a surface-oxygenated PdNiMnO porous film. The Mn-doping was designed to promote surface oxygenation using a facile anodization process that created sufficiently exposed interfaces between Pd and the support, strengthening the SMSI effects at the Pd/oxygenated support interface for enhancing ORR performance. Furthermore, the Ni-containing oxygenated catalyst served as both the active component for the oxygen evolution reaction (OER) and the functional support for stabilizing Pd, making PdNiMnO a bifunctional catalyst for zinc–air flow batteries (ZAFB). As a proof-of-concept, the ZAFB (PdNiMnO) shows a maximal power density of 211.6 mW cm –2 and outstanding cycling stability for over 2000 h with a minimal voltage gap of 0.69 V at a current density of 10 mA cm –2 , superior to the state-of-the-art catalysts.

25 ENERGY STORAGE↗

Enabling technologies for the continuous electrically driven conversion of CO 2 and water to multi-carbon products at high current densities

Here, we demonstrate greatly improved conversion of CO 2 using a gas diffusion electrode (GDE) with flowing electrolyte configuration for CO 2 gas delivery in combination with a high surface area nickel phosphide electrocatalyst. This configuration achieves 40–50% selectivity for total carbon products over H 2 formation (HER) at total current densities ranging from 50 to 300 mA cm -2 . We developed a soft-templating method using CTAB detergent micelles for synthesis of phase-pure Ni 2 P, achieving a 260-fold larger surface area (BET) and porous sponge-like morphology that produces stable currents. This catalyst produces mainly one C-product, methylglyoxal (MG, C 3 H 4 O 2 ) with 38–47% overall selectivity, the highest reported selectivity for a 12-electron reduction product. The versatile soft-templating method for electrocatalyst synthesis uses low-temperature (185 °C) that is permissive for incorporation of co-catalysts that are otherwise destroyed by the high temperatures used in traditional solid-state synthesis (SSS). The non-porous Ni 2 P-SSS catalyst produces mainly H 2 at these current densities. Achieving these high currents and C/H selectivity benefits from use of hydrophobic polymers as co-catalyst binders (cationic = Nafion, anionic = PFAEM and neutral = PTFE) to improve CO 2 conversion. PFAEM is the better ionomer for the CO 2 RR at high current density, postulated as due to suppressing CO 2 conversion to inactive bicarbonate. Precipitation of the carbon products as a polycarbonate polymer occurs at high currents.

36 MATERIALS SCIENCE↗

Effect of Computational Schemes on Coupled Flow and Geo-Mechanical Modeling of CO 2 Leakage through a Compromised Well

Carbon capture, utilization, and storage (CCUS) describes a set of technically viable processes to separate carbon dioxide (CO 2 ) from industrial byproduct streams and inject it into deep geologic formations for long-term storage. Legacy wells located within the spatial domain of new injection and production activities represent potential pathways for fluids (i.e., CO 2 and aqueous phase) to leak through compromised components (e.g., through fractures or micro-annulus pathways). The finite element (FE) method is a well-established numerical approach to simulate the coupling between multi-phase fluid flow and solid phase deformation interactions that occur in a compromised well system. We assumed the spatial domain consists of a three-phases system: a solid, liquid, and gas phase. For flow in the two fluids phases, we considered two sets of primary variables: the first considering capillary pressure and gas pressure (PP) scheme, and the second considering liquid pressure and gas saturation (PS) scheme. Fluid phases were coupled with the solid phase using the full coupling (i.e., monolithic coupling) and iterative coupling (i.e., sequential coupling) approaches. The challenge of achieving numerical stability in the coupled formulation in heterogeneous media was addressed using the mass lumping and the upwinding techniques. Numerical results were compared with three benchmark problems to assess the performance of coupled FE solutions: 1D Terzaghi’s consolidation, Liakopoulos experiments, and the Kueper and Frind experiments. We found good agreement between our results and the three benchmark problems. For the Kueper and Frind test, the PP scheme successfully captured the observed experimental response of the non-aqueous phase infiltration, in contrast to the PS scheme. These exercises demonstrate the importance of fluid phase primary variable selection for heterogeneous porous media. We then applied the developed model to the hypothetical case of leakage along a compromised well representing a heterogeneous media. Considering the mass lumping and the upwinding techniques, both the monotonic and the sequential coupling provided identical results, but mass lumping was needed to avoid numerical instabilities in the sequential coupling. Additionally, in the monolithic coupling, the magnitude of primary variables in the coupled solution without mass lumping and the upwinding is higher, which is essential for the risk-based analyses.

deformation flow↗

Cellular fluidics

The natural world provides many examples of multiphase transport and reaction processes that have been optimized by evolution. These phenomena take place at multiple length and time scales and typically include gas–liquid–solid interfaces and capillary phenomena in porous media. Many biological and living systems have evolved to optimize fluidic transport. However, living things are exceptionally complex and very difficult to replicate, and human-made microfluidic devices (which are typically planar and enclosed) are highly limited for multiphase process engineering. In this paper, we introduce the concept of cellular fluidics: a platform of unit-cell-based, three-dimensional structures—enabled by emerging 3D printing methods—for the deterministic control of multiphase flow, transport and reaction processes. We show that flow in these structures can be ‘programmed’ through architected design of cell type, size and relative density. We demonstrate gas–liquid transport processes such as transpiration and absorption, using evaporative cooling and CO 2 capture as examples. We design and demonstrate preferential liquid and gas transport pathways in three-dimensional cellular fluidic devices with capillary-driven and actively pumped liquid flow, and present examples of selective metallization of pre-programmed patterns. Our results show that the design and fabrication of architected cellular materials, coupled with analytical and numerical predictions of steady-state and dynamic behaviour of multiphase interfaces, provide deterministic control of fluidic transport in three dimensions. Cellular fluidics may transform the design space for spatial and temporal control of multiphase transport and reaction processes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗