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Griffin: A MOOSE-based reactor physics application for multiphysics simulation of advanced nuclear reactors

Griffin is a Multiphysics Object-Oriented Simulation Environment (MOOSE) based reactor physics application for multiphysics simulations of advanced reactor designs jointly developed by Idaho National Laboratory and Argonne National Laboratory. This paper summarizes the motivation, significance, architecture, design, and features of Griffin. Griffin offers flexible and extensible features to address the challenges associated with advanced reactor designs. These features range from fundamental particle transport to specific reactor physics tasks. The features cover a wide range including on-the-fly and traditional two-step cross-section generation methods, steady-state and transient transport solvers suitable for both heterogeneous and homogeneous models, high-fidelity depletion where thousands of isotopes can be tracked and low-fidelity depletion characterized by burnup, etc. The most fundamental aspect that sets Griffin apart from other reactor analysis codes is that it is developed based on the MOOSE framework. A modular development approach is strongly enforced, with multiphysics being an essential element considered since the beginning of Griffin’s development. Griffin links various MOOSE physics modules and couples to other MOOSE-based applications and non-MOOSE-based applications for multiphyiscs simulations. Griffin includes three modules: ISOXML for preparing and managing multigroup cross sections, radiation transport for solving the neutron transport equation, and reactor analysis for user-oriented reactor physics analysis functionalities. Griffin uses various finite element methods for spatial discretization, multigroup approximation for energy discretization and discrete ordinates method, spherical harmonics expansion method, and diffusion approximation for streaming direction discretization to solve the neutron transport equation. Griffin’s flexibility is evidenced through Griffin’s various applications to fast reactor, high-temperature reactor, pebble bed reactor, molten salt reactor, and microreactor designs. Griffin development follows the software quality assurance procedure for MOOSE-based applications and with software requirements consistent with the ASME NQA-1 standard. Griffin has been adopted into the reactor analysis system for the U.S. NRC and is in use at U.S. companies, universities and national laboratories.

97 MATHEMATICS AND COMPUTING↗

Polar Bear™ – Innovative Capture of Storage Tank Vapors

Polar Bear™ is a patented technology developed by the Energy & Environmental Research Center (EERC) to capture storage tank vapors and eliminate methane emissions from upstream oil- and gas-producing facilities. Sparked by early commercial investment, the EERC licensed the technology and extended the intellectual property to storage tanks. Polar Bear™ is uniquely engineered and adapted to individual lower-producing facilities where there is otherwise no economic alternative for capturing tank vapors. A high number of small producing oil and gas wells are distributed across the country. The aggregate contributes to a significant volume of emissions. Because of the lack of economy of scale, gas volumes from these facilities are typically not recovered and contribute to methane emissions. Polar Bear™ provides a fit-for-purpose compression solution that addresses cost by reducing complexity with respect to conventional vapor recovery units and eliminating oil changes. Unique to Polar Bear™ is the capability to separate oxygenated gas from storage tank vapors. Storage tanks are designed to “breathe,” allowing gas to enter and escape during internal level and temperature changes. This infiltration of air into the tank headspace imparts undesirable oxygen content with respect to pipeline gathering. Polar Bear™ separates the vapor stream, allowing oxygen-rich gas to be used as fuel on-site while recovering the liquids-rich portion of the gas where oxygen content is minimized. A prototype system was tested to verify process models, evaluate operational performance, and advance the technology readiness level from 5 to 6. Results provide a good match between experimental measurements and process models, indicating the models are useful for future scale-up and field design. Various mixtures of nitrogen and liquefied petroleum gas were tested to understand the mass balance of nitrogen and how it relates to the potential control of oxygen content. Findings indicate that less than 2000 ppm of oxygen is likely to remain in the liquid portion of the gas in field applications. The research and development prepare the technology for field implementation to eliminate routine and fugitive methane emissions from storage tanks.

02 PETROLEUM↗

Impact of Hydrogen on Methane and Pollutant Emissions over Three-Way Catalysts with Natural Gas–Hydrogen Blends

Blending natural gas (NG) with hydrogen (H₂) can improve combustion and engine performance while potentially facilitating the catalytic conversion of methane and other pollutants, resulting in cleaner tailpipe emissions. This study evaluates the impact of H2 on the conversion of methane, CO, and NOx emissions on a commercial three-way catalyst (TWC) in a flow reactor using synthetic gas mixtures that simulate stoichiometric engine exhausts with NG or NG+H₂ combustion. The work examines whether, and how, the additional amount of H₂ in the exhaust stream affects the conversion efficiency of methane and other pollutants. Experiments were conducted with both degreened and aged catalysts under controlled conditions, systematically varying temperature, the air-to-fuel equivalence ratio (λ), and λ modulation. Test conditions covered λ values from 0.996 to 1.000 to represent nominally stoichiometric engine operation with different λ modulation amplitudes, as well as a range of temperatures to inform control strategies for effective CH₄, CO, and NOₓ reduction. Overall, the results show that hydrogen addition significantly improves the conversion efficiency of CH₄ and NOₓ, particularly at temperatures below 500 °C. More significantly, this study highlights that exhaust gas composition, operating temperature, λ management, and the oxygen storage capacity of the TWC all play major roles in affecting the tailpipe emissions from NG and NG+H₂ combustion.

Prikhodko, Vitaly [ORNL] (ORCID:0000000244685836)↗

The ever-evolving active site: transformation of single atoms to extended structures during the Rh-catalyzed reverse water–gas shift reaction

At low temperatures (< 400°C), single atoms of Rh supported on rutile TiO 2 (rTiO 2 ) are responsible for the formation of CO during the reverse water gas shift (RWGS), while methane production is associated with the Rh-TiO 2 interface due to the correlation between methane formation rates and the volume-averaged Rh nanoparticle diameter. As the temperature is increased to >540°C, there is a notable increase in CO selectivity and methane production rates tend towards zero. The time to reach zero depends on the temperature but independent of the initial Rh structure (single atoms and/or nanoparticles), which is controlled by the catalyst preparation method (wetness impregnation versus colloidal nanoparticles). At 600°C and > 4 h time on stream, the catalytic behaviour becomes completely agnostic to the initial Rh structure as well as weight loading, and the catalysts are highly selective for the reverse water gas-shift reaction. Post-reaction HR-TEM image analysis confirms Rh nanoparticles crystallize/order during the reaction; at 400°C, most of the Rh particles are disordered, while at 600°C, they are more ordered (i.e., development of defined faceting). Infrared spectroscopy of CO adsorption on Rh nanoparticles confirms the appearance of defined facets after annealing in nitrogen at high temperatures. Annealing the Rh/rTiO 2 catalysts prior to the RWGS reaction demonstrates the structural transformation of Rh depends only on time and temperature and not on reactant or product fugacity. Sites responsible for stabilizing Rh single atoms are no longer competent at higher temperatures, enabling their integration into existent nanoparticles. As the reaction temperature is increased to temperatures >540°C, the dominant active site for CO production evolves from single atoms to extended Rh structures.

36 MATERIALS SCIENCE↗

Preliminary Testing of a Continuous Cryopump for Primary Fusion Device Pumping and Direct Internal Recycling

Here, the concept of directly recirculating fusion machine exhaust gas, bypassing the tritium plant, to make fuel pellets was proposed in the 1990s and later termed direct internal recycling (DIR). In the DIR concept, the residual fusion fuel in the machine exhaust stream is separated from impurities locally and diverted directly to the fueling systems, bypassing isotopic separation and other processing equipment, and therefore significantly reducing the required size of the fuel processing plant, reducing plant inventory, and thus increasing the economic viability of fusion as an energy source. One concept for DIR consists of a series of cryogenic pumps to separate the impurities from the machine exhaust gas using different triple point temperatures and saturation curves of exhaust constituents. In this concept, the plasma exhaust is initially passed through an impurity trap operating at ~25–30 K to desublimate impurities such as hydrocarbons, argon, oxygen, and nitrogen. The resulting process stream will consist of DT fuel and helium. The process stream is then pumped by a continuous cryopump known as a “snail pump.” This pump is a steady-state continuous cryopump that desublimates all remaining exhaust gas constituents while allowing helium, a byproduct of the fusion reaction, to pass through. The helium is pumped to the tritium plant for processing while the desublimated material is continuously scraped off, heated up, and transported to the fueling system. This article will present the cryogenic DIR concept and outline the design and operation of the snail pump, along with results from preliminary testing. Tests to assess pumping and separation efficiency found that at D2 flows below 50.7 Pa ⋅ m3/s with 1% helium, the pump is capable of pumping and separating the gas with a resulting DIR fraction of >99%, with no helium entrained in the primary fuel exhaust stream. The main limitation is due to the thermal performance of the cryogenic circuits of the pump, which will be addressed in future testing.

Gebhart III, Trey E. [Oak Ridge National Laborator↗

Photocatalytic Semi‐Hydrogenation of Acetylene to Polymer‐Grade Ethylene with Molecular and Metal–Organic Framework Cobaloximes

Abstract The semi‐hydrogenation of acetylene in ethylene‐rich gas streams is a high‐priority industrial chemical reaction for producing polymer‐grade ethylene. Traditional thermocatalytic routes for acetylene reduction to ethylene, despite progress, still require high temperatures and high H 2 consumption, possess relatively low selectivity, and use a noble metal catalyst. Light‐powered strategies are starting to emerge, given that they have the potential to use directly the abundant and sustainable solar irradiation, but are ineffective. Here an efficient, >99.9% selective, visible‐light powered, catalytic conversion of acetylene to ethylene is reported. The catalyst is a homogeneous molecular cobaloxime that operates in tandem with a photosensitizer at room temperature and bypasses the use of non‐environmentally friendly and flammable H 2 gas feed. The reaction proceeds through a cobalt‐hydride intermediate with ≈100% conversion of acetylene under competitive (ethylene co‐feed) conditions after only 50 min, and with no evolution of H 2 or over‐hydrogenation to ethane. The cobaloxime is further incorporated as a linker in a metal–organic framework; the result is a heterogeneous catalyst for the conversion of acetylene under competitive (ethylene co‐feed) conditions that can be recycled up to six times and remains catalytically active for 48 h, before significant loss of performance is observed.

Stone, Aaron E. B. S.↗

Pyrogenic Organic Matter Laboratory Experiment: Aerobic Respiration and Geochemistry from Variably Inundated Stream Sediments (v3)

This dataset supports a broader study examining the effects of variable inundation and pyrogenic organic matter on ecosystem respiration. The dataset provides data generated from a laboratory batch experiment investigating the interaction between variable inundation conditions (wet and dry sediment) and pyrogenic organic matter (burned and unburned treatments). The contents include time series dissolved oxygen, sediment geochemistry data, and field metadata (including qualitative information on instream and river corridor characteristics). This data package was originally published in November 2025. It was updated in April 2026 (v2; new and modified files) and May 2026 (v3; modified files). See the change history section in the readme for more details For details on how to navigate data packages generated by this project, see https://data.ess-dive.lbl.gov/portals/PNNLRiverCorridorSFA/About. In addition to a readme, this data package also includes a file-level metadata (FLMD) file that describes each file and a data dictionary (DD) that describes all column/row headers and variable definitions. This dataset is comprised of (1) file-level metadata; (2) data dictionary; (3) field metadata; (4) international generic sample number (IGSN) mapping file; (5) readme; (6) field protocol; (7) sample name metadata; (8) an environmental context picture for the dry and inundated sampling locations; and (9) a subfolder with sample data from the sediment incubation experiment. The sample data subfolder contains (1) dissolved organic carbon (DOC, measured as non-purgeable organic carbon, NPOC); (2) total nitrogen (TN); (3) gravimetric moisture; (4) partial pressure and production rates of carbon dioxide, methane, and nitrous oxide; (5) field wet sediment mass, dry sediment mass, water mass, and field wet sediment volume in incubation and sediment NPOC/TN vials; (6) methods codes; (7) respiration rates, pH, and temperature from after the incubation, raw time series dissolved oxygen and temperature, and a subfolder containing associated plots and scripts; (8) ions; (9) FTICR-MS methods; and (10) a subfolder of 12 Tesla (12T) FTICR-MS data. This folder contains the CoreMS processed data and three subfolders, one containing the .xml files, one containing the CoreMS output files, and the other containing instructions and scripts for processing the files in CoreMS (https://github.com/EMSL-Computing/CoreMS). All files are .csv, .pdf, .R, .xml, .html, .Rmd, .py, .cal, .json, or .jpg.

54 ENVIRONMENTAL SCIENCES↗

Experimental Characterization of High-Surface Area Thermal Energy Storage

There is growing interest in energy storage technologies due to the expansion of renewable energy sources that are inherently intermittent and the increasing frequency of extreme weather events that disturb the power grid. Power consumption in buildings makes up approximately 76% of all electricity usage on the grid and is primarily used for thermal applications such as space conditioning, hot water, and cooking. This makes thermal energy storage (TES) an ideal solution for many of these applications. Many TES technologies rely on latent energy storage, which utilizes the melting/solidification of phase change materials (PCM) to store energy. Typically, TES designs suffer from low power density due to their low inherent thermal conductivity. This limitation makes the deployment of TES in active applications difficult as the ease of access to energy is essential for effective use. Common routes for improving power density include high thermal conductivity additives or extended features such as fins that increase cost. This study presents an alternative approach to improving performance through increasing the overall surface area to volume ratio of the device, to increase the available area for convection to occur between the working fluid and PCM. In the study a commercial PCM was selected with a transition temperature ideal for space heating applications. The heat exchanger design utilizes a unique application of triply periodic minimal surfaces (TPMS) for macro-encapsulation of the PCM. The use of TPMS for heat exchangers has been growing in interest due to their high-surface area to volume ratios, which were previously unmanufacturable until the development of additive manufacturing. A modular system was designed and manufactured with a stereolithography resin printing system that is then backfilled with PCM. An experiment test set-up is designed to test the charge and discharge performance of the thermal storage using a conditioned air stream. The pressure drop of the design is tested across a variety of flow rates. When compared to existing experimental data within literature, there is excellent agreement based on the Reynolds number at similar hydraulic diameters. Several inlet temperatures are tested at consistent temperature differences from the phase change temperature for both charging and discharging. Additionally, the volumetric flow rate is varied for each temperature set point. It was found that increasing flow rate had diminishing returns in reducing the overall charge time of the TES. The temperature delta from the melting temperature was the primary contributor to the change in average heat flux with limited variation in average heat transfer rate between charging and discharging at similar inlet temperatures and flow rates. The TPMS heat exchanger design has a high air-side pressure drop but it provides high heat transfer rates. This helps maintain a high outlet temperature during discharge, which is important to thermal comfort applications. The design, manufacturing, and experimental characterization of the TES device will be presented as part of this study.

25 ENERGY STORAGE↗

A Rapid Procedure Development Approach for Multi-stage Validation of Novel Nuclear Power Plant Systems

The integration of renewable energy sources into the modern grid introduces variability in generation, challenging nuclear reactors to remain economically viable amid low wholesale electricity prices. To address this, Idaho National Laboratory?s Flexible Plant Operation and Generation program explores alternative revenue streams, including commoditizing excess thermal energy. A Thermal Power Dispatch (TPD) system enables steam extraction from the secondary loop for industrial uses like hydrogen production via high-temperature steam electrolysis.

99 - GENERAL AND MISCELLANEOUS↗

Understanding and tuning organocatalysts for versatile condensation polymer deconstruction

Plastics are widely used for their durability and versatility, but recycling remains a major challenge, especially for mixed or contaminated waste. Mechanical recycling works well for clean, single-polymer streams like PET but has limited efficiency for complex waste streams. Chemical recycling, particularly glycolysis, is often employed to selectively deconstruct condensation polymers under mild conditions. This study explores catalyst design for glycolysis using linear free energy (Hammett) analysis to evaluate how catalyst structure influences polymer deconstruction. Polycaprolactone (PCL) is used as a model polyester due to its solubility and low deconstruction temperature. Triazabicyclodecene (TBD) paired with benzoic acid derivatives depicts a clear linear trend in depolymerization rates with Hammett values. TBD with p-aminobenzoic acid (PABA) stands out for its catalytic efficiency, thermal stability, and scalability, along with PABA's commercial availability as vitamin B-10. The TBD : PABA catalyst not only effectively breaks down PCL but also enables sequential deconstruction of polycarbonate, PET, and Nylon in mixed waste streams. These results highlight the value of Hammett-guided catalyst design and establish TBD : PABA as a promising, scalable organocatalyst for mixed plastic recycling, enabling recovery of individual polymer building blocks from blended waste and offering a practical route toward circular plastics.

Zheng, Jackie [Univ. of Tennessee, Knoxville, TN (↗

Dual-Bed Radioiodine Capture from Complex Gas Streams with Zeolites: Regeneration and Reuse of Primary Sorbent Beds for Sustainable Waste Management

Dual-sorbent systems are proposed for radioiodine management with a regenerated primary bed for multiple cycles of use in complex conditions and a secondary bed for disposal with higher waste loadings. Sorbent approaches for the effective capture of gaseous radioiodine (isotopes 129 I and 131 I) produced from a range of nuclear processes have been studied for over half a century. (1−5) Whether or not a sorbent (e.g., molecular sieve) is required to physically screen/trap or chemically bind a radionuclide of interest through chemisorption, the complexity of the gas stream has a large impact on the performance (e.g., loading capacity, selectivity) and active life of a sorbent bed. (3) Silver mordenite (AgZ), the U.S. Department of Energy baseline sorbent for radioiodine capture from nuclear processes, performs well within acidic conditions and at elevated temperatures (6) and can be consolidated into a chemically durable waste form for long-term disposal. (7,8) However, new sorbents are being sought because optimal capture performance of AgZ significantly decreases in dynamic oxidizing environments with competing species, and it is expensive and it contains Ag (a toxic metal). (9) Until a new sorbent is found to replace AgZ, the regeneration and reuse of AgZ is an attractive alternative to a single-use primary sorbent bed. In this regard, a primary sorbent could be designed for enhanced capture in complex gas streams and the ability to be regenerated for reuse. Here, a secondary sorbent could then be tailored for maximum iodine loading in the gas stream and chemical durability within a disposal facility.

chemisorption↗

Permanent Stress Adaptation and Unexpected High Light Tolerance in the Shade-Adapted Chlamydomonas priscui

The Antarctic photopsychrophile, Chlamydomonas priscui UWO241, is adapted to extreme environmental conditions, including permanent low temperatures, high salt, and shade. During long-term exposure to this extreme habitat, UWO241 appears to have lost several short-term mechanisms in favor of constitutive protection against environmental stress. This study investigated the physiological and growth responses of UWO241 to high-light conditions, evaluating the impacts of long-term acclimation to high light, low temperature, and high salinity on its ability to manage short-term photoinhibition. We found that UWO241 significantly increased its growth rate and photosynthetic activity at growth irradiances far exceeding native light conditions. Furthermore, UWO241 exhibited robust protection against short-term photoinhibition, particularly in photosystem I. Lastly, pre-acclimation to high light or low temperatures, but not high salinity, enhanced photoinhibition tolerance. These findings extend our understanding of stress tolerance in extremophilic algae. In the past 2 decades, climate change-related increasing glacial stream flow has perturbed long-term stable conditions, which has been associated with lake level rise, the thinning of ice covers, and the expansion of ice-free perimeters, leading to perturbations in light and salinity conditions. Our findings have implications for phytoplankton survival and the response to change scenarios in the light-limited environment of Antarctic ice-covered lakes.

Plant Sciences↗

Data, model inputs, and analysis scripts associated with a manuscript on stream intermittency controls across spatial scales in Pacific Northwest watersheds

NOTE: The manuscript associated with this data package is currently in review. The data may be revised based on reviewer feedback. Upon manuscript acceptance, this data package will be updated with the final dataset and additional metadata. This data package is associated with the manuscript "Hydroclimatic Memory and Watershed Template Shape Stream Intermittency: Multi-scale Attribution Using Process-based Simulation and Explainable ML" by Niroula et al. (2026), submitted to Water Resources Research (WRR). The study investigates the dominant controls on stream intermittency across local, reach, and watershed scales using a coupled process-based simulation and explainable machine-learning framework. Long-term daily simulations from the Advanced Terrestrial Simulator (ATS) were used to generate wetness states and ponded-depth responses over river-corridor cells. These ATS outputs were then aggregated across scales and used to train XGBoost (eXtreme Gradient Boosting) models. SHAP (SHapley Additive exPlanations) was applied to quantify the relative importance of hydroclimatic forcings, watershed template attributes, and antecedent-memory effects in shaping intermittency behavior. The analysis is carried out for three contrasting Pacific Northwest watersheds: Oak Creek (OCW), American River Watershed (ARW), and H.J. Andrews (HJA). Across these testbeds, the package contains ATS-ready watershed inputs, ATS run configuration and selected output files, model-evaluation data products, intermittency-analysis datasets, machine-learning target-feature tables, SHAP outputs, and notebooks used to organize, analyze, and visualize results. At a high level, the package documents a workflow in which ATS provides the physically based simulation backbone and explainable machine learning is used as a post-processing attribution tool. The contents are intended to support interpretation of the manuscript figures and results, provide context for how intermittency metrics were generated at multiple scales, and preserve the key artifacts needed to understand and reuse the analysis workflow. The package contains a high-level directory summary file (`summary.txt`) and four main content folders (1) `evaluation_plots` contains evaluation figures and supporting evaluation datasets; (2) `intermittency_plots` contains intermittency-focused analysis notebook and prepared datasets; (3) `ml-training-and-shap_values_plots` contains ML training inputs, SHAP outputs, and figure-generation notebooks; and (4) `watershed_mesh_and_ats_input` contains ATS model setup materials, forcing inputs, geometry, and selected run files. More specifically, the `evaluation_plots` folder contains the notebook used for ATS evaluation plotting and site-specific evaluation datasets. These include evapotranspiration and water-balance products for three watersheds, as well as an Oak Creek field-measurement discharge file. The `intermittency_plots` folder contains the notebook used for intermittency analysis and the prepared datasets used to analyze intermittent and non-intermittent wetness behavior across the study watersheds. The `ml-training-and-shap_values_plots` folder contains notebooks and outputs for the machine-learning and explainability workflow. This includes the main XGBoost and SHAP notebook(s), a beeswarm plotting notebook, target-feature tables for machine-learning training, SHAP summary tables, and per-sample SHAP value archives. The `watershed_mesh_and_ats_input` folder contains ATS-related watershed inputs and supporting materials. This includes mesh and shape products, ATS-readable LAI and meteorological forcing inputs, selected ATS spinup and transient-run files, and a watershed workflow example notebook. Subdirectories are organized by watershed where applicable.All files are .cpg (codepage files), .csv (comma-separated values), .dbf (database files), .exo (Exodus mesh format), .h5 (HDF5 format), .ipynb (Jupyter notebooks), .pkl (Python pickle), .prj (projection files), .sh (shell scripts), .shp (shapefile geometry), .shx (shapefile index), .txt (text files), or .xml (markup data).

Advanced Terrestrial Simulator↗

Distinctive Pattern of Global Warming in Ocean Heat Content

Abstract Huge heat anomalies in the atmosphere and ocean in recent years are not yet explained. Strong characteristic patterns in temperatures for upper layers of the ocean occurred from 2000 to 2023 in the presence of global warming from increasing atmospheric greenhouse gases. Here, we show that the deep tropics are warming, although sharply modulated by El Niño–Southern Oscillation events, with strong heating in the extratropics near 40°N and 40°–45°S but little heating near 20°N and 25°–30°S. The heating is most clearly manifested in zonal-mean ocean heat content and is evident in sea surface temperatures. The strongest heating is in the Southern Hemisphere, where aerosol effects are small. Estimates are made of the contributions to heating of top-of-atmosphere (TOA) radiation, atmospheric energy transports, surface fluxes of energy, and redistribution of energy by surface winds and ocean currents. The patterns of change are not directly related to TOA radiation but are evident in net surface energy fluxes and inferred ocean heat transports, underscoring their coupled origin. Changes in the atmospheric circulation through a poleward shift in ocean jet streams and storm tracks are reflected in surface wind-driven ocean Ekman transports. As well as human-induced climate change, internal natural variability is likely in play. Hence, the atmosphere and ocean currents are systematically redistributing heat from global warming, profoundly affecting local climates. Significance Statement As the climate changes, it has been difficult to discern meaningful patterns. Distinctive patterns of change have occurred in the ocean when examined as zonal averages around latitude bands. Most excess heat from global warming resides in the ocean and, since 2005, has become focused into bands near 40°N and 40°S, with little net warming in the subtropics. The strongest warming is in the Southern Hemisphere, although sea surface temperatures have increased more in the Northern Hemisphere. Changes in the atmospheric circulation through a poleward shift in the jet stream and storm tracks are primarily responsible along with corresponding changes in ocean currents. These changes are linked through surface exchanges of energy via heat, moisture, and wind stress.

Trenberth, Kevin E. [National Center for Atmospher↗

Stable Co-valorization of Carbon Dioxide and Methane via Dynamic Reconstruction of a Metal Oxide Solid Solution Catalyst

Dry reforming of methane (DRM) is a process that converts two greenhouse gases (methane and carbon dioxide) into syngas, a mixture of H 2 and CO, that can lead to a variety of value-added chemicals. Owing to its endothermic nature, high reaction temperatures up to 800 °C are typically required and the grand challenge lies in developing robust catalysts without sintering and coking-induced deactivation during the long-term on-stream operation. Towards this aim, herein, a robust complex oxide-supported NiCu alloy catalyst was generated in situ during DRM. By leveraging the configurational stability of a solid oxide solution precursor, tightly anchored NiCu bimetallic nanoparticles were in situ exsoluted and acted as the active sites in DRM. The as-afforded catalyst exhibited stable performance for DRM due to the ability to repel coke off the surface as the reaction proceeds. Kinetic experiments along with top surface characterization detail the reconstruction behavior of the solid oxide solution under DRM reaction conditions. In conclusion, the fundamental insights from this work provide guidance on generating resistant and flexible catalysts via in situ active sites formation from easily synthesized metal oxide solid solutions.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Mercury Testing with Sludge Batch 10 Tank 40 Simulant

Savannah River Mission Completion (SRMC) requested that researchers at Savannah River National Laboratory (SRNL) perform testing designed to examine why the Defense Waste Processing Facility (DWPF) is not collecting elemental mercury in the Mercury Water Wash Tank (MWWT). In order for DWPF to recover mercury, mercuric oxide must first be reduced to elemental mercury. The elemental mercury must then be steam stripped, condense, and coalesce in the Mercury Water Wash Tank (MWWT) during chemical processing in the Sludge Receipt and Adjustment Tank (SRAT). The efficiency of these steps was investigated in a series of laboratory scale SRAT experiments under the nitric-glycolic and nitric-formic flowsheets utilizing Momentive Y-17112 and Antifoam 747. Mercury speciation in the Slurry Mix Evaporator Condensate Tank (SMECT) and condensate streams was also examined. The key conclusions from these experiments are as follows: Mercury II Oxide may not be fully reduced to elemental mercury during acid addition at 93°C. Higher temperatures, i.e., boiling may be necessary to fully reduce Mercury II Oxide. The highest percent mercury recovery (71 %) in the MWWT was observed in the MS-NGA-17112 experiment (nitric-glycolic acid flowsheet with Momentive Y-17112), which is how DWPF is currently operating the SRAT.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Solar Thermochemical Carbon Dioxide Splitting Using Ceria and Iron Aluminate Foam Devices and Simulation of a Plant System for Demonstration

An international research project has been undertaken to integrate a unique solar thermal processing reactor system with ceria and iron aluminate as active redox materials for CO2 splitting. Experimental investigations for CO2 splitting were conducted using a solar simulator and tube furnace at Niigata University, followed by demonstrations using a high-flux solar furnace (HFSF) at the National Renewable Energy Laboratory (NREL) in Golden, CO. Each experimental setup consisted of foam devices composed of reticulated porous ceramic (RPC). The RPC has a full ceria or iron aluminate body. It fabricated using the replica method and subjected to a two-step redox reaction, which iteratively separated a stream of CO2 into O2 and CO. Reactivity was evaluated using CO production per mass of the reactive material. The tubular furnace yielded a CO production of 6.41 mL/g at a reduction temperature of 1600degrees C, showcasing a higher CO production rate and total amount than those obtained from experiments conducted with solar simulators and solar furnace setups. For iron aluminate RPC, the productivity was measured as 3.57 mL/g using HFSF at a reduction temperature of 1450degrees C. These results are somewhat higher than those of the previous experiment at lower reduction temperatures of 1400degrees C-1500degrees C. Additionally, the production of CO in the case of ceria RPC was compared with the steady flow model simulation, which assumed chemical equilibrium at various levels of oxygen partial pressure during the reduction process. On the basis of these results, this study proposes a solar fuel system with an open receiver that uses a high-temperature heat transfer fluid.

carbon dioxide thermochemical splitting↗

Effects of Recovery Conditions and Aggregation Mechanisms on the Chemical and Physical Properties of Hybrid Poplar and Corn Stover Lignins

Heterogeneity in the physical properties and processing behavior of lignins recovered from biorefining process streams can hinder their effective utilization and industrial valorization. This work investigates lignin recovery by acidification from alkaline pretreatment liquors of varying sources (corn stover and hybrid poplar), compositions, solid contents, and incubation temperatures prior to filtration. Recovered lignins were characterized for filtration performance, mass yield, chemical composition, particle size and morphology, and color. A transition temperature was identified corresponding to marked shifts in lignin physical properties and was a function of the solid content and liquor source. Filtration below this temperature yielded slow-filtering, dark, brittle lignins with smoother particle surfaces, whereas precipitation above this threshold yielded fast-filtering, lighter, powdery lignins with rougher particle surfaces. The impact of temperature and concentration on universal cluster aggregation mechanisms was proposed to explain the differences between lignin particle properties and filtration behavior.

Aggregation↗