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DOE OSTI2016

Effects of Lewis acidity of metal oxide promoters on the activity and selectivity of Co-based Fischer–Tropsch synthesis catalysts

Metal oxides of Ce, Gd, La, Mn, and Zr were investigated as promoters for improving the activity and selectivity of Co-based FTS catalysts. The extent to which these promoters decrease the selectivity toward CH 4 and increase the selectivity toward C 5+ hydrocarbons was found to depend on both the loading and the composition of the oxide promoter. Elemental mapping by STEM–EDS revealed that the propensity for a given metal oxide to associate with Co affects the sensitivity of the product distribution to changes in promoter loading. For all promoters, a sufficiently high loading resulted in the product distributions becoming insensitive to further increases in promoter loading, very likely due to the formation of a half monolayer of promoter oxide over the Co surface. Simulations suggest that the fraction of Co active sites that are adjacent to the promoter moieties approaches unity at this degree of coverage. The oxidation state of the promoter metal cation under reaction conditions, determined by in situ XANES measurements, was used to calculate relative Lewis acidity of the promoter metal cation. A strong positive correlation was found between the C 5+ product selectivity and the Lewis acidity of the promoter metal cations, suggesting that the promotional effects are a consequence of Lewis acid–base interactions between the reaction intermediates and the promoter metal cations. Rate data obtained at different pressures were used to estimate the apparent rate coefficient and the CO adsorption constant appearing in the Langmuir–Hinshelwood expression that describes the CO consumption kinetics for both unpromoted and the metal oxide-promoted catalysts. Both parameters exhibited positive correlations with the promoter Lewis acidity. In conclusion, these results are consistent with the hypothesis that the metal cations of the promoter act as Lewis acids that interact with the O atom of adsorbed CO to facilitate CO adsorption and dissociation.

Johnson, Gregory R.↗

DOE OSTI2018

Contamination control monitoring at the Los Alamos National Laboratory’s Plutonium Facility

Plutonium airborne contamination creates a particular hazard because of the possibility of intake by inhalation. To preclude excursions of radioactive materials into the operator’s breathing zone, controls are used to prevent contamination. Measures to control radioactive contamination include eliminating or minimizing the spread of contamination and preventing cross-contamination. Contamination control philosophy at the plutonium facility is conveyed in one simple statement: Detect the contamination closest to the source as possible! Speed and distance when self-monitoring is critical to detecting plutonium contamination. Responding correctly to an alarm or monitor not working properly minimizes the consequences of plutonium contamination. Performing a full body frisking correctly and using the Peerchecking tool also minimize the consequences of plutonium contamination.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

DOE OSTI2014

The iterative thermal emission method: A more implicit modification of IMC

For over 40 years, the Implicit Monte Carlo (IMC) method has been used to solve challenging problems in thermal radiative transfer. These problems typically contain regions that are optically thick and diffusive, as a consequence of the high degree of “pseudo-scattering” introduced to model the absorption and reemission of photons from a tightly-coupled, radiating material. IMC has several well-known features that could be improved: a) it can be prohibitively computationally expensive, b) it introduces statistical noise into the material and radiation temperatures, which may be problematic in multiphysics simulations, and c) under certain conditions, solutions can be nonphysical, in that they violate a maximum principle, where IMC-calculated temperatures can be greater than the maximum temperature used to drive the problem. We have developed a variant of IMC called iterative thermal emission IMC, which is designed to have a reduced parameter space in which the maximum principle is violated. ITE IMC is a more implicit version of IMC in that it uses the information obtained from a series of IMC photon histories to improve the estimate for the end of time step material temperature during a time step. A better estimate of the end of time step material temperature allows for a more implicit estimate of other temperature-dependent quantities: opacity, heat capacity, Fleck factor (probability that a photon absorbed during a time step is not reemitted) and the Planckian emission source. We have verified the ITE IMC method against 0-D and 1-D analytic solutions and problems from the literature. These results are compared with traditional IMC. We perform an infinite medium stability analysis of ITE IMC and show that it is slightly more numerically stable than traditional IMC. We find that significantly larger time steps can be used with ITE IMC without violating the maximum principle, especially in problems with non-linear material properties. The ITE IMC method does however yield solutions with larger variance because each sub-step uses a different Fleck factor (even at equilibrium)

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2023

Stress characterization for friction-stir-welded electric vehicle battery trays with application of neutron diffraction

The battery tray is an essential component that protects and controls battery-cell temperatures in electric and plug-in hybrid vehicles. The functional stress limit of the battery tray heavily depends on the residual stress acquired from the manufacturing process. Consequently, exceeding the stress limit of the battery tray during operation could compromise the battery-cell banks and may risk the vehicle's safety. Hence, understanding residual stress formation is vital for design and safety concerns. Here, in the current study, AA 6061-plates were friction stir welded to an A365 high-pressure die-cast battery tray to create sealed coolant channels in the battery tray. However, this multi-material lap friction stir weld introduces residual stress into the battery tray, resulting in distortion. This distortion was mitigated using burnishing or coining operations, though straightening the battery tray had initially unknown effects on the residual stress. Therefore, neutron diffraction was utilized to characterize residual stresses after straightening. The results indicate that the friction stir welding (FSW) operation generated residual stresses exceeding the yield strength of the material, consequently deforming the battery tray by ±3 mm from the pre-weld geometry. The burnishing operation reduced the residual stresses below the material's yield strength while restoring the tray to within ±0.75 mm of the pre-weld geometry. Similarly, the coining operation restored the battery tray to within ±0.75 mm of the pre-weld geometry, however, increasing the number of locations where the residual stress exceeds the yield strength of the material.

36 MATERIALS SCIENCE↗

DOE OSTI2018

A novel approach to quantifying the kinetics of point defect absorption at dislocations

We report that microstructure evolution under creep loading and/or irradiation is largely affected by the two-way coupling between dislocation induced plasticity and point defect diffusion as mediated by the internal elastic strain field within the medium. The magnitude of this effect has been quantified only in idealized, simplified environments such that estimates of absorption rates of point defects to dislocations ignore the collective effects on capture rates arising from particular distribution of dislocations in a given network, the interaction of point defects with the internal strain, or in many cases both. To quantify these effects, we advance a novel methodology to determine point defect capture rates locally within a spatially resolved finite difference solution to the diffusion problem for arbitrarily directed dislocations and the corresponding strain fields. In addition to examining the effects of these couplings on local and effective absorption rates of dislocation networks, the potential consequences of these interactions on other microstructure evolution phenomena are examined using void swelling under irradiation as an example. Our study indicates that local rates of defect mediated microstructural changes such as cavity growth can vary strongly as a consequence of the arrangement of the dislocation network and the corresponding strain state. Lastly, the heterogeneous aspects of the resultant defect populations are shown to provide mechanisms for microstructural evolution under irradiation that are not available in the conventional homogeneous theory.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Evaluation of HVAC & refrigeration system fault behaviors and impacts: A systematic review

Achieving the goals of green buildings critically depends on the fault-free operation of heating, ventilation and air conditioning and refrigeration (HVAC&R) systems. However, faults frequently occur in these systems, causing a range of negative consequences, including increased energy consumption, diminished operational performance, compromised indoor environmental quality, higher operational costs, and shortened system lifespan. The evaluation of fault behaviors and impacts plays a critical role in revealing fault characteristics and consequently supports many research areas, including the design of the high-performance equipment, development of fault detection and diagnostics (FDD) and robust control approaches, as well as the enhancement of maintenance decision-making activities. This paper systematically reviews 112 research publications that reported the analysis and evaluation of fault behaviors and impacts in HVAC&R systems over the past thirty years. Here, we designed a review approach to address five crucial research questions, namely: 1) the objectives of analysis and evaluation of fault behaviors and impacts, 2) data sources, 3) equipment/system types and fault types, 4) evaluation methods including evaluation measures and associated metrics, and 5) challenges and future directions in the research on evaluating of fault behaviors and impacts. In-depth discussions on these questions help bridge the gap between the evaluation of fault behaviors and impacts and their practical applications, such as the development of high-performance systems, fault models, FDD methods, and maintenance decision-making tools within the HVAC&R FDD domain.

Chen, Yimin [Oak Ridge National Laboratory (ORNL),↗

DOE OSTI2018

Towards understanding HPC users and systems: A NERSC case study

High performance computing (HPC) scheduling landscape currently faces new challenges due to thechanges in the workload. Previously, HPC centers were dominated by tightly coupled MPI jobs. HPCworkloads increasingly include high-throughput, data-intensive, and stream-processing applications. Asa consequence, workloads are becoming more diverse at both application and job levels, posing newchallenges to classical HPC schedulers. There is a need to understand the current HPC workloads andtheir evolution to facilitate informed future scheduling research and enable efficient scheduling in futureHPC systems.In this paper, we present a methodology to characterize workloads and assess their heterogeneity,at a particular time period and its evolution over time. We apply this methodology to the workloads ofthree systems (Hopper, Edison, and Carver) at the National Energy Research Scientific Computing Center(NERSC). We present the resulting characterization of jobs, queues, heterogeneity, and performance thatincludes detailed information of a year of workload (2014) and evolution through the systems’ lifetime(2010–2014).

Rodrigo, Gonzalo P.↗

DOE OSTI2015

The effect of postprocessing on tensile property and microstructure evolution of friction stir welding aluminum alloy joint

Friction stir welding is an efficient manufacturing method for joining aluminum alloy and can dramatically reduce grain size conferring excellent plastic deformation properties. Consequently, friction stir welding is used to manufacture tailor welded blanks to optimize weight or performance in the final component. In the study, the microstructural evolution and mechanical properties of friction stir welding joint during plastic forming and subsequent heat treatment were investigated. The microstructural characteristics of the friction stir welding joints were studied by Electron Backscattered Diffraction and Transmission Electron Microscopy. The mechanical properties were evaluated by tensile and microhardness tests. It is found that the tensile and yield strengths of friction stir welding joints are significantly improved after severe plastic deformation due to the grain refinement. Following heat treatment, the strength of the friction stir welding joints significantly decrease due to the obvious abnormal grain growth. Careful attention must be given to the processing route of any friction stir welding joint intended for plastic forming, especially the annealing between forming passes. Severe plastic deforming of the friction stir welding joint leads to a high level of stored energy/dislocation density, which causes the abnormal grain growth during subsequent heat treatment, and consequently reduce the mechanical properties of the friction stir welding joint. - Highlights: • Great changes are observed in the microstructure of FSW joint after postprocessing. • Postprocessing shows great effect on the microstructure stability of FSW joint. • The weld shows more significant decrease in strength than the BM due to the AGG. • Attention must be given to the processing route of FSW joint for plastic forming.

36 MATERIALS SCIENCE↗

DOE OSTI2017

Effect of small addition of Cr on stability of retained austenite in high carbon steel

High carbon steels with dual phase structures of martensite and austenite have considerable potential for industrial application in high abrasion environments due to their hardness, strength and relatively low cost. To design cost effective high carbon steels with superior properties, it is crucial to identify the effect of Chromium (Cr) on the stability of retained austenite (RA) and to fully understand its effect on solid-state phase transition. This study addresses this important knowledge gap. Using standard compression tests on bulk material, quantitative X-ray diffraction analysis, nano-indentation on individual austenitic grains, transmission electron microscopy and electron backscatter diffraction–based orientation microscopy techniques, the authors investigated the effect of Cr on the microstructure, transformation behaviour and mechanical stability of retained austenite in high carbon steel, with varying Cr contents. The results revealed that increasing the Cr %, altered the morphology of the RA and increased its stability, consequently, increasing the critical pressure for martensitic transformation. This study has critically addressed the elastoplastic behaviour of retained austenite – and provides a deep understanding of the effect of small additions of Cr on the metastable austenite of high carbon steel from the macro- to nano-level. Consequently, it paves the way for new applications for high carbon low alloy steels. - Highlights: • Effect of small addition of Cr on metastable austenite of high carbon steel from the macro- to nano-level • A multi-scale study of elastoplastic behaviour of retained austenite in high carbon steel • The mechanical stability of retained austenite during plastic deformation increased with increasing Cr content • Effect of grain boundary misorientation angle on hardness of individual retained austenite grains in high carbon steel.

36 MATERIALS SCIENCE↗

DOE OSTI2018

ECCI based characterization of dislocation shear in polycrystalline arrays during heterogeneous deformation of commercially pure titanium

A new electron channeling contrast imaging (ECCI) based approach for the characterization of heterogeneous plastic deformation across multiple grains in a polycrystal is presented. The nature of the shear accommodation at grain boundaries has been assessed by evaluating the spatial distribution of dislocations and slip system activities near the boundaries and relating these observations to standard slip transfer criteria and the global state of stress. The direction of slip band propagation, and consequently the location of dislocation slip band nucleation, was determined by characterizing the slip band widths across individual grains. This assessment leads to a better understanding of the factors involved in polycrystalline deformation, including the grain boundary shear accommodation associated with both dislocation pile-ups and grain boundary dislocation nucleation. Because ECCI allows study of dislocation structures over large surface areas, and thus larger overall volumes than typically are accessible by other techniques, the overall approach allows the dislocation distribution across individual grains to be understood in terms of the broader polycrystalline constraints.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Macrovoid resolved simulations of transport through HPRO relevant membrane geometries

Modeling the transport properties such as diffusivity and permeability of high pressure reverse osmosis (HPRO) membranes is critical for the selection and manufacture of membranes suitable for operation under high pressure. These properties can be significantly affected by the changes in heterogeneous pore structures due to compaction. Here, the modeling platform presented in this work resolves the two scale porosity in HPRO relevant membranes. A synthetic membrane geometry is constructed based on available experimental visualizations of pore structures. The simulations directly capture the flow channeling that results from a combination of material properties and geometric features of the macrovoids. A parametric study is presented to account for the transition of flow characteristics from a material governed regime to a macrovoid governed regime. Permeability of the membrane is evaluated using the simulation data and compared with an existing model that scales with the square of tortuosity over a range of material properties. The model is found to perform well under a narrow range of tortuosity while deviating from the calculated permeabilities at extreme conditions. The effective permeability of the membrane is found to vary by at least two orders of magnitude between the two flow regimes. It is also observed that tortuosity is a bounded property with its upper limit determined by the macrovoid geometry. Consequently, the tortuosity based correlations fail near a flow regime that is mainly governed by the macrovoids. The modeled permeability can be more than an order of magnitude smaller than the simulation result. A new model based on flux-weighted porosity of a membrane is introduced and its correlation with tortuosity is studied. The model agrees with the simulated data as, in addition to tortuosity, it also accounts for the flux partition within and outside the flow channels. Such correlations enable extending the existing understanding of flow characteristics to enhance predictability of porous media models.

42 ENGINEERING↗

DOE OSTI2020

Utilizing ink composition to tune bulk-electrode gas transport, performance, and operational robustness for a Fe-N-C catalyst in polymer electrolyte fuel cell

With lower site density and turnover frequency, platinum group metal (PGM)-free catalysts based electrodes are often greater than 50 mu m thick in order to increase performance across the fuel cell operating range. Consequently, PGM-free electrodes have an additional bulk electrode transport resistance beyond the local or aggregate level transport in thin platinum-based electrodes. In parallel to the development of more active and durable PGM-free catalysts, advancements in understanding the interplay between PGM-free electrode fabrication, bulk-electrode transport, proton conductivity and performance are needed. Here, the relationship between ionic and gas phase transport through the electrode thickness is modified by adjusting electrocatalyst and ionomer flocculation/interaction at the ink level. The influence of the ink composition (water/n-propanol content) is examined via various in-situ electrochemical and ex-situ characterization techniques and the resulting electrode structure/performance relationship contrasted with electrode performance robustness across a range of relative humidity (RH). For the electrocatalyst examined here, a water-rich (82 wt% H2O) ink formulation was favorable for operation at high RH due to improved molecular diffusion through larger electrode pores. In contrast, the improved interactions between ionomer and electrocatalyst enabled a more robust electrode and higher performance during low RH operation for the 50 wt% H2O content ink.

08 HYDROGEN↗

DOE OSTI2021

Multicriterion benefit evaluation methodology for safety enhancements in nuclear power plants and application for FLEX strategies

Here we propose a multicriterion benefit evaluation (MCBE) methodology for evaluating costs and benefits of implementing safety enhancements in nuclear power plants. The MCBE methodology establishes a comprehensive evaluation scope using multiple evaluation criteria (including public risk, occupational risk, plant revenue, and plant cost) and multiple contexts (including plant normal operations, incidents, and accidents). The MCBE methodology formulates a benefit or cost element as the product of a monetary consequence and its occurrence-likelihood change. The MCBE methodology also incorporates a decision maker’ preferences toward occurrence likelihood and monetary consequence into cost and benefit estimations through a modified usage of cumulative prospect theory. This paper applies the MCBE methodology to the implementation of diverse and flexible coping strategy (FLEX) in a generic nuclear power plant as an illustrative example. The FLEX benefits are evaluated through three types of influence paths: plant safety enhancement, risk-informed activities, and potential additional credit of FLEX in supporting plant operation and maintenance-efficiency improvement. The benefit-to-cost ratio (BCR) of FLEX implementation is calculated. Sensitivity analyses are conducted to examine the impacts of modeling assumptions and input parameter values on the BCR.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

DOE OSTI2021

Full core LOCA safety analysis for a PWR containing high burnup fuel

For economic reasons, the US nuclear industry is renewing efforts to build a technical basis to extend peak rod average burnup limits above the current regulatory burnup limit of 62 GWd/MTU. The primary driver of these efforts is to economically increase pressurized water reactor (PWR) cycle lengths to 24 months, reduce the number of fresh fuel assemblies, increase time online, thereby reducing number of outages and their associated cost, higher fuel utilization, and possibly reduce core design constraints. In order for US nuclear utilities to leverage these economic efficiencies, the US Nuclear Regulatory Commission (NRC) will likely require nuclear power plants (NPPs) to analyze a number of potential operational occurrences and their potential consequences with each new core design prior to resuming normal operation. Potential operational occurrences can be divided into three primary regimes: (1) normal operation, (2) anticipated operation occurrences (AOOs), and (3) design basis accidents (DBAs). Normal plant operation is an operating regime in which the plant operates within specified operational limits until the end of the cycle, whereas AOOs are events that result in the NPP deviating outside the normal operating regime. A key attribute of an AOO is that the occurrence should be expected. However, by definition, the occurrence of an AOO does not result in significant impact to critical safety functions. The last potential operational occurrence is a DBA. From the fuel performance point-of-view, DBAs can be subdivided into two bounding categories: (1) loss of coolant accidents (LOCAs), and (2) reactivity insertion accidents (RIAs). Unlike AOOs, DBAs may result in fuel rod failure. The NRC imposes fundamental acceptance criteria to minimize radiological consequences to the public and onsite staff. Furthermore, safety criteria are typically linked to the fulfillment of other acceptance criteria related to reactor safety equipment designed to mitigate DBAs.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2022

Metal fuel relocation experiments with pressure injection

A pool-type sodium-cooled fast reactor (SFR) using metal fuels has a number of inherent safety features that can support benign consequences for design basis accidents (DBAs). Even in postulated severe accident conditions, the core is designed to remain under sub-critical condition in a passive coolable geometry. In case of the postulated severe accidents in SFRs, fuel relocation in the core region along the coolant channel is an important negative reactivity feedback factor that lowers the reactor power level and consequently eliminates the possibility of recriticality. Therefore, understanding the relocation behavior of fuels and the coolability of the relocated fuels in the postulated severe accident is one of the most important factors in the safety assessment of SFRs. In the present study, the relocation behavior of the metal fuel in a pin bundle geometry was investigated by injecting the metal fuels into the coolant channels with pressure. The first metal fuel relocation with pressure injection (RPI-1) experiment showed that many of the metal fuels levitated to upper plenum. In case of RPI-2 experiment, the Real Time X-ray Video System (RTXVS) was constructed and used to obtain a real time X-ray video of the experiment. This real time X-ray video clearly showed the relocation behavior of the pressure injected metallic uranium in the sodium coolant channel. Through this video, it was confirmed that part of the fuel was dispersed downward and part of the fuel was dispersed upward, and the relocation behavior of the injected fuel proceeded simultaneously in the downward and upward directions. So, it can be concluded that in case of pressure injection of the metallic fuel, there is a possibility that the metallic fuel can be quickly removed from the core region, resulting in a negative reactivity feedback effect.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2016

Climate teleconnections and indicators of coastal systems response

This article surveys secular urban sandy beaches erosion – accretion and its relationship with climate teleconnections, e.g., El Niño Southern Oscillation (ENSO), Atlantic Multidecadal Oscillation (AMO), and extreme events, e.g., storm surges, great rivers' floods, and heavy rains in adjacent basins. The paper aims to discuss these issues and the expected coastal retreat as a consequence of manmade climate changes, e.g., sea level rise (SLR) and increased storminess in the coming decades. Several beaches (Buceo, Malvín, Pocitos, Ramírez) and two tidal creek sandy mouths (Carrasco and Pando), with different characteristics but all constrained by coastal linear infrastructure were studied. These sites are located along the urbanised coast of the middle region of Río de la Plata microtidal river estuary. All of them show a more or less strong retreat trend with alternated fluctuations, e.g., weak retreat likely due to sea level rise, significant erosion very likely due to storm surges, and processes of loss of sediment stock, as well as episodes of sand recovery. Therefore, these beaches require interventions to preserve their beach prism and dry sand surface. In search for answers to better understand why and under what conditions the process of advance and retreat of the coastline occur, we have analysed different teleconnections and carried out reanalyses for wind anomalies during ENSO events from 1951 to 2010. Both weak and moderate erosion–accretion periods are likely related to atmospheric anomalies, e.g., wind direction changes and the consequent swell and littoral drift changes, related to El Niño and La Niña events. The former associated with accretion and the latter with erosion. In the past most interventions have been reactive. Increased knowledge of climate and weather relationship with the sedimentary balance provides an approach that would allow developing beach risk-management, pro-active strategies and climate adaption measures focused on the generation and recovery planning based on the analysis of the occurrence and prediction of El Niño/La Niña events.

Oceanography↗

DOE OSTI2024

Urbanization exacerbates continental- to regional-scale warming

Urbanization is usually ignored when estimating past changes in large-scale climate and for future climate projections since cities historically covered a small fraction of the Earth’s surface. Here, by combining global land surface temperature observations with historical estimates of urban area, we demonstrate that the urban contribution to continental- to regional-scale warming has become non-negligible, especially for rapidly urbanizing regions and countries in Asia. Consequently, expected urban expansion over the next century suggests further increased urban influence on large-scale surface climate in the future (approximately 0.16 K for North America and Europe for high-emission scenario in 2100). Based on these results, also seen for air temperature, we argue that, in line with other forms of land use/land cover change, urbanization should be explicitly included in climate change assessments. This requires incorporation of dynamic urban extent and biophysics in current-generation Earth system models to quantify potential urban feedback on the climate system across scales.

Chakraborty, TC↗

DOE OSTI2018

Understanding land use change impacts on microclimate using Weather Research and Forecasting (WRF) model

To explore potential climatic consequences of land cover change in the Kolkata Metropolitan Development area, we projected microclimate conditions in this area using the Weather Research and Forecasting (WRF) model driven by future land use scenarios. Specifically, we considered two land conversion scenarios including an urbanization scenario that all the wetlands and croplands would be converted to built-up areas, and an irrigation expansion scenario in which all wetlands and dry croplands would be replaced by irrigated croplands. Results indicated that land use and land cover (LULC) change would dramatically increase regional temperature in this area under the urbanization scenario, but expanded irrigation tended to have a cooling effect. In the urbanization scenario, precipitation center tended to move eastward and lead to increased rainfall in eastern parts of this region. Increased irrigation stimulated rainfall in central and eastern areas but reduced rainfall in southwestern and northwestern parts of the study area. This study also demonstrated that urbanization significantly reduced latent heat fluxes and albedo of land surface; while increased sensible heat flux changes following urbanization suggested that developed land surfaces mainly acted as heat sources. In this study, climate change projection not only predicts future spatiotemporal patterns of multiple climate factors, but also provides valuable insights into policy making related to land use management, water resource management, and agriculture management to adapt and mitigate future climate changes in this populous region. (C) 2017 Elsevier Ltd. All rights reserved.

AIR-QUALITY↗