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DOE OSTI2016

Dry Reforming of Ethane and Butane with CO 2 over PtNi/CeO 2 Bimetallic Catalysts

Dry reforming is a potential process to convert CO 2 and light alkanes into syngas (H 2 and CO), which can be subsequently transformed to chemicals and fuels. Here in this work, PtNi bimetallic catalysts have been investigated for dry reforming of ethane and butane using both model surfaces and supported powder catalysts. The PtNi bimetallic catalyst shows an improvement in both activity and stability as compared to the corresponding monometallic catalysts. The formation of PtNi alloy and the partial reduction of Ce 4+ to Ce 3+ under reaction conditions are demonstrated by in-situ Ambient Pressure X-ray Photoemission Spectroscopy (AP-XPS), X-ray Diffraction (XRD) and X-ray Absorption Fine Structure (XAFS) measurements. A Pt-rich bimetallic surface is revealed by Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS) following CO adsorption. Combined in-situ experimental results and Density Functional Theory (DFT) calculations suggest that the Pt-rich PtNi bimetallic surface structure would weaken the binding of surface oxygenates/carbon species and reduce the activation energy for C-C bond scission, leading to an enhanced dry reforming activity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

The Impact of Slantwise Descending Dry Intrusions on the Marine Boundary Layer and Air-Sea Interface Over the ARM Eastern North Atlantic Site

Dry intrusions (DIs) are synoptic-scale slantwise descending airstreams from the midlatitude upper troposphere toward the boundary layer at lower latitudes. Typically occurring behind cold fronts, such intrusions of dry air often reach the boundary layer and cause its deepening, thereby affecting boundary-layer clouds. Although subsidence is generally an inherent feature of the subtropical marine boundary layer (MBL), it is unclear how the MBL reacts to the transient, dynamically distinct DI. In this study, reanalysis data were combined with observations from the Atmospheric Radiation Measurement Eastern North Atlantic (ENA) site (39.1 degrees N,28.0 degrees W) to characterize the impact of DIs on MBL characteristics and clouds. Specifically, an objective criterion is applied to the observations made during the winter months of 2016-2018 to identify the DI days from those before and following DIs, and reference periods without DIs. The analyses suggest substantial deepening of the well-mixed boundary layer accompanied by changes in the cloud, precipitation and thermodynamic properties during the DI events. During the DI, the lower troposphere cooled and dried substantially thereby inducing strong surface sensible and latent heat fluxes. All while a strong inversion builds up at the elevated MBL top affecting cloud occurrence. The results show DIs to affect the boundary layer and cloud structure at the ENA site similar to 21% of the time in winter months, with the response of the cloud fields to the DI-fronts substantially different than that to the non-DI fronts. Hence, the DI events should be considered while studying boundary layer and cloud processes in the region.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2013

Development of a novel ultrasonic temperature probe for long-term monitoring of dry cask storage systems

With the recent cancellation of the Yucca Mountain repository and the limited availability of wet storage utilities for spent nuclear fuel (SNF), more attention has been directed toward dry cask storage systems (DCSSs) for long-term storage of SNF. Consequently, more stringent guidelines have been issued for the aging management of dry storage facilities that necessitate monitoring of the conditions of DCSSs. Continuous health monitoring of DCSSs based on temperature variations is one viable method for assessing the integrity of the system. In the present work, a novel ultrasonic temperature probe (UTP) is being tested for long-term online temperature monitoring of DCSSs. Its performance was evaluated and compared with type N thermocouple (NTC) and resistance temperature detector (RTD) using a small-scale dry storage canister mockup. Our preliminary results demonstrate that the UTP system developed at Argonne is able to achieve better than 0.8 Degree-Sign C accuracy, tested at temperatures of up to 400 Degree-Sign C. The temperature resolution is limited only by the sampling rate of the current system. The flexibility of the probe allows conforming to complex geometries thus making the sensor particularly suited to measurement scenarios where access is limited.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2014

Preparation of polyaniline/sodium alanate hybrid using a spray-drying process

Nowadays, hydrogen is highly interesting as an energy source, in particular in the automotive field. In fact, hydrogen is attractive as a fuel because it prevents air pollution and greenhouse emissions. One of the main problems with the utilization of hydrogen as a fuel is its on-board storage. The purpouse of this work was to develop a new hybrid material consisting of a polyaniline matrix with sodium alanate (NaAlH{sub 4}) using a spray-drying process. The polyaniline used for this experiment was synthesized by following a well-established method for the synthesis of the emeraldine base form of polyaniline using dodecylbenzenesulfonic acid as dopant. Micro particles of polyaniline/sodium alanate hybrids with 30 and 50 wt% of sodium alanate were prepared by using a spray-drying technique. Dilute solutions of polyaniline/sodium alanate were first prepared, 10g of the solid materials were mixed with 350 ml of toluene under stirring at room temperature for 24h and the solutions were dried using spray-dryer (Büchi, Switzerland) with 115°C of an inlet temperature. The hybrids were analyzed by differential scanning calorimetry, FT-IR and scanning electron microscopy (SEM). The addition of sodium alanate decreased the glass transition temperature of the hybrids when compared to neat polyaniline. FT-IR spectrum analysis was performed to identify the bonding environment of the synthesized material and was observed that simply physically mixture occurred between polyaniline and sodium alanate. The SEM images of the hybrids showed the formation of microspheres with sodium alanate dispersed in the polymer matrix.

08 HYDROGEN↗

DOE OSTI2017

Provitamin A biofortification of cassava enhances shelf life but reduces dry matter content of storage roots due to altered carbon partitioning into starch

Storage roots of cassava (Manihot esculenta Crantz), a major subsistence crop of sub-Saharan Africa, are calorie rich but deficient in essential micronutrients, including provitamin A bcarotene. In this study, b-carotene concentrations in cassava storage roots were enhanced by coexpression of transgenes for deoxy-D-xylulose-5-phosphate synthase (DXS) and bacterial phytoene synthase (crtB), mediated by the patatin-type 1 promoter. Storage roots harvested from field-grown plants accumulated carotenoids to ≤50 lg/g DW, 15- to 20-fold increases relative to roots from nontransgenic plants. Approximately 85%–90% of these carotenoids accumulated as all-trans-b-carotene, the most nutritionally efficacious carotenoid. b-Caroteneaccumulating storage roots displayed delayed onset of postharvest physiological deterioration, a major constraint limiting utilization of cassava products. Large metabolite changes were detected in b-carotene-enhanced storage roots. Most significantly, an inverse correlation was observed between b-carotene and dry matter content, with reductions of 50%–60% of dry matter content in the highest carotenoid-accumulating storage roots of different cultivars. Further analysis confirmed a concomitant reduction in starch content and increased levels of total fatty acids, triacylglycerols, soluble sugars and abscisic acid. Potato engineered to co-express DXS and crtB displayed a similar correlation between b-carotene accumulation, reduced dry matter and starch content and elevated oil and soluble sugars in tubers. Transcriptome analyses revealed a reduced expression of genes involved in starch biosynthesis including ADP-glucose pyrophosphorylase genes in transgenic, carotene-accumulating cassava roots relative to nontransgenic roots. These findings highlight unintended metabolic consequences of provitamin A biofortification of starch-rich organs and point to strategies for redirecting metabolic flux to restore starch production.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Adjoint sensitivity analysis and data assimilation for verification of dry storage cask contents

Dry cask storage is a method for interim storage of spent fuel assemblies which contain fissile isotopes of uranium and plutonium. These can present a proliferation concern and consequently there is a need for non-destructive testing methods to verify a dry cask's contents for proliferation protection. We present an application of adjoint sensitivity analysis and data assimilation to a multigroup diffusion model of dry cask storage. Adjoint sensitivity analysis allows the efficient calculation of sensitivities for use in data assimilation to calibrate imprecisely known parameter values and data consistency tests to detect diversion scenarios. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2026

The Interactions Between Shading and Organic Fertilizer Application on Dry-farmed Tomato Grown Between Photovoltaic Panels

Agrivoltaic systems are mixed systems of solar photovoltaic (PV) panels and agricultural production, where shade from the panels can result in lower evapotranspiration for crops, which is of particular interest for dryland agriculture. Dry-farmed tomato (Solanum lycopersicum) production in the Willamette Valley of Oregon has lower total yields and higher rates of blossom-end rot (BER) than irrigated tomato production, resulting in reduced marketable yields. To determine how dry-farmed ‘Early Girl’ tomato performed in an agrivoltaics system, a trial was conducted at the Valley Creek Solar Project (Salem, OR, USA) in 2020, using three different amendment treatments and three levels of shading from the panels. Amendment treatments were 0N (receiving no fertilizer), 84N (receiving 84 kg·ha −1 N), and 168N (receiving 168 kg·ha −1 N), applied as processed chicken manure. Plants were estimated to receive an irradiance factor of 30%, 76%, and 89% for full-shade, partial-shade, and full-sun treatments respectively. There was an interaction between amendment treatments and shading treatments in their effects on unblemished yield (yield of fruit without BER or sunscald). The optimum fertilizer application for full-shade and partial-shade rows was 84N, the optimum for full-sun rows was 0N. Fertilizing these rows at these rates resulted in an unblemished yield for the aisle of 11.1 t·ha −1 , which was lower than unblemished yields reported in previous experiments and trials in open fields. However, these results are from a single location and a single year, and other solar sites may behave more similar to open-field conditions. Shading from the panels increased average fruit weight and decreased incidence of BER and sunscald, suggesting that crops were less drought stressed. This resulted in similar unblemished yields for the full-shade and full-sun plots at 84N and 168N. Applying fertilizer resulted in higher total yields, smaller average fruit weight, increased BER incidence, and decreased sunscald incidence. The results suggest a possible synergy between dry-farmed tomato production and agrivoltaics, although several concerns remain, including difficulties managing the vegetation under panels, rules restricting PVs on high-value agricultural soils, and the possibility of soil compaction during PV installation.

14 SOLAR ENERGY↗

DOE OSTI2013

Viability of Existing INL Facilities for Dry Storage Cask Handling

This report evaluates existing capabilities at the INL to determine if a practical and cost effective method could be developed for opening and handling full-sized dry storage casks. The Idaho Nuclear Technology and Engineering Center (INTEC) CPP-603, Irradiated Spent Fuel Storage Facility, provides the infrastructure to support handling and examining casks and their contents. Based on a reasonable set of assumptions, it is possible to receive, open, inspect, remove samples, close, and reseal large bolted-lid dry storage casks at the INL. The capability can also be used to open and inspect casks that were last examined at the TAN Hot Shop over ten years ago. The Castor V/21 and REA-2023 casks can provide additional confirmatory information regarding the extended performance of low-burnup (<45 GWD/MTU) used nuclear fuel. Once a dry storage cask is opened inside CPP-603, used fuel retrieved from the cask can be packaged in a shipping cask, and sent to a laboratory for testing. Testing at the INL’s Materials and Fuels Complex (MFC) can occur starting with shipment of samples from CPP-603 over an on-site road, avoiding the need to use public highways. This reduces cost and reduces the risk to the public. The full suite of characterization methods needed to establish the condition of the fuel exists and MFC. Many other testing capabilities also exist at MFC, but when those capabilities are not adequate, samples can be prepared and shipped to other laboratories for testing. This report discusses how the casks would be handled, what work needs to be done to ready the facilities/capabilities, and what the work will cost.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2023

Preheating of Cold, High Moisture Particulate Biomaterials to Reduce Drying Time

Forest Concepts led a two-year project to reduce fossil fuel consumption and improve the energy efficiency of dryers through the application of radio frequency (RF) energy impartation to preheat cold-wet bulk particulate biomass materials. A comprehensive biomass heating and drying mathematical model was developed that enables simulation of drying systems for biomass as well as most other bulk porous particulate materials. Experimental and modeling results conclude that energy consumption for both RF preheating and hot-air preheating are essentially equal for cold, high-moisture feedstocks that are above fiber saturation and therefore not economically beneficial for those conditions. Further results suggest that RF heating may have a direct energy consumption benefit in the late stages of drying and in case of preheating biomass that has a moisture content below fiber saturation. This work was funded in part by the US Department of Energy under contact DE-EE0009130.

09 BIOMASS FUELS↗

DOE OSTI2022

Melting Behavior of Conventional and Hydrogen-Reduced DRI in a Simulated EAF Steel Bath

The melting behavior of carbon-free direct reduced iron (DRI) produced by hydrogen reduction has been investigated in a simulated electric arc furnace (EAF) melting environment. A testing apparatus was created to document the melting rates under various bath conditions in slag and steel. This investigation is specific to pellets melted in a steel bath. A model was developed to simulate the shell growth and melting rate of a non-reactive DRI pellet in molten steel. Data acquired from preliminary experiments are utilized to validate the model. This investigation sheds light on the potential effects of melting hydrogen-reduced DRI in the EAF.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Taxonomic and Functional Diversity of Aquatic Macroinvertebrate Assemblages and Water Quality in Rivers of the Dry Tropics of Costa Rica

One of Costa Rica’s driest areas is the province of Guanacaste, in the Pacific Northwest, with almost no rain during the dry season from November to April. Due to this marked seasonality, the area is covered by dry tropical deciduous forest, considered the most threatened and least known tropical ecosystem in this area. This study analyzes and characterizes the assemblages of aquatic macroinvertebrates in water bodies within the Tempisque basin. Biological water quality was measured using the BMWP′-CR index. Macroinvertebrate assemblages were analyzed using abundance, richness, and functional feeding group approaches (FFG). Partial least square (PLS) analyses were performed, and the relationships between environmental factors and macroinvertebrate assemblages are also discussed. Macroinvertebrate assemblages were dominated numerically by mayflies, caddisflies, flies, and beetles. The BWMP′-CR index showed varying biological water quality, ranging from “very bad” to “excellent,” depending on rainfall and site management. Results suggest that tropical Mesoamerican rivers contradict the “river continuum concept” because predators and scrapers displace shredders in numbers. On the other hand, the study area shows a notable high richness of the Coleoptera genera. The class Rhynchocoela (Nemertea) is reported for the first time in Central America. The results indicate that the dry forest river ecosystem shows staggering biodiversity despite the surrounding agricultural land use, probably because of their older origin concerning tropical rain forests in Central America.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Testing Various Cement Formulations under Temperature Cycles and Drying Shrinkage for Low-Temperature Geothermal Wells

Low-enthalpy geothermal wells are considered a sustainable energy source, particularly for district heating in the Netherlands. The cement sheath in these wells experiences thermal cycles. The stability of cement recipes under such conditions is not well understood. In this work, thermal cycling experiments for intermediate- and low-temperature geothermal well cements have been conducted. The samples were cured either under ambient conditions or under realistic pressure and temperature for 7 days. The samples did not show any signs of failure after performing 10 cycles of thermal treatment between 100 °C and 18 °C. We also tested cement formulations under drying conditions. Drying shrinkage is caused by a reduction in the water content of cement, which leads to capillary forces that can damage cement. Such circumstances lead to tensile stresses causing radial cracks. Most samples exhibited cracks under low humidity conditions (drying). Fiber reinforcement, especially using short PP fibers, improved the cement’s resilience to temperature and humidity changes. Such additives can improve the longevity of cement sheaths in geothermal wells.

36 MATERIALS SCIENCE↗

NASA NTRS2021

Evaluation of SO2, SO4(2−) and an Updated SO2 Dry Deposition Parameterization in the United Kingdom Earth System Model

In this study we evaluate simulated surface SO2 and sulphate (SO4(2-)) concentrations from the United Kingdom Earth System Model (UKESM1) against observations from ground based measurement networks in the USA and Europe for the period 1987 to 2014. We find that UKESM1 captures the historical trend for decreasing concentrations of atmospheric SO2 and SO4(2-) in both Europe and the USA over the period 1987 to 2014. However, in the polluted regions of the eastern USA and Europe, UKESM1 over-predicts surface SO2 concentrations by a factor of 3, while under-predicting surface SO4(2-) concentrations by 25-35%. In the cleaner western USA, the model over-predicts both surface SO2 and SO4(2-) concentrations by a factor of 12 and 1.5 respectively. We find that UKESM1’s bias in surface SO2 and SO4(2-) concentrations is variable according to region and season. We also evaluate UKESM1 against total column SO2 from the Ozone Monitoring Instrument (OMI) using an updated data product. This comparison provides information about the model’s global performance, finding that UKESM1 over predicts total column SO2 over much of the globe, including the large source regions of India, China, the USA and Europe as well as over outflow regions. Finally, we assess the impact of a more realistic treatment of the model’s SO2 dry deposition parameterization. This change increases SO2 dry deposition to the land and ocean surfaces, thus reducing the atmospheric loading of SO2 and SO(sup 2-)(sub 4). In comparison with the ground-based and satellite observations, we find that the modified parameterization reduces the models over prediction of surface SO2 concentrations and total column SO2. Relative to the ground-based observations the simulated surface SO4(2-) concentrations are also reduced, while the simulated SO2 dry deposition fluxes increase.

SO2↗

DOE OSTI2013

Viability of Existing INL Facilities for Dry Storage Cask Handling

INL, dry storage cask, Idaho National Lab, Long Te↗

DOE OSTI2018

Radiography of Dry Cask Storage for Used Nuclear Fuel

Since the U.S. currently only approves of storing used nuclear fuel in pools or dry casks, the demand for dry cask storage is on the rise due to the continuous operation of currently existing nuclear plants which are reaching or have reached the capacity of their used fuel pools. With the rising demand comes additional pressure to ensure the integrity of dry cask systems. Visual inspection is costly and man-power intensive, so alternative nondestructive testing techniques are desired to insure the continued safe and effective storage of fuel. Several approaches being investigated by the University of Florida and the larger multi-university Department of Energy (DOE) Nuclear Energy University Program (NEUP) Integrated Research Project (IRP) are gamma or neutron radiography, both transmission based and interior source emission. Additionally muon radiography is discussed. This work leverages the well-established techniques in medical image reconstruction and applies them to a significantly larger scale with additional considerations due to the dense nuclear materials which serves as effective shields for radiation. Emission source radiography relies on the radiation that is emitted from the used fuel. The main advantage of this technique is the passive nature of the measurement. The fuel is already emitting radiation and only detectors are needed. Transmission radiography uses an external source of radiation to penetrate the side of the cask. Challenges include selecting the external source spectrum to avoid overlap with the spectrum emitted from the fuel, and ensuring the radiation dose limits do not exceed those mandated by the Nuclear Regulatory Commission (NRC). Benefits of this technique include better understanding of the source location allowing for clear image reconstruction, and isolation of the signal from surrounding radiation sources. Muon radiography takes advantage of the natural background flux coming from the interaction of the atmosphere with cosmic radiation. The technique is particularly effective at interrogating large dense objects as the highly energetic muons have smaller cross sections than most typical sources and energies used in nuclear engineering. The various techniques are discussed individually then the conclusion compares them. Finally, future work is identified.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2020

ASNF Engineering Scale Drying Experiment System Operability Functional Requirements

This checklist specifies the functional requirements for the drying system installed at Holtec International under the scope of INL Contract # 215725, in collaboration with University of South Carolina under INL Contract Number 207046, consistent with the parameters described in INL/EXT-19-56017, Aluminum-clad Spent Nuclear Fuel Engineering Scale Drying Experiment Design. Completion of the ASNF Engineering Scale Drying Experiment Acceptance Criteria for Fabricated Items, INL/MIS-20-58551, is a prerequisite.

36 MATERIALS SCIENCE↗

DOE OSTI2013

Demonstrating the Safety of Long-Term Dry Storage - 13468

Commercial nuclear plants in the United States were originally designed with the expectation that used nuclear fuel would be moved directly from the reactor pools and transported off site for either reprocessing or direct geologic disposal. However, Federal programs intended to meet this expectation were never able to develop the capability to remove used fuel from reactor sites - and these programs remain stalled to this day. Therefore, in the 1980's, with reactor pools reaching capacity limits, industry began developing dry cask storage technology to provide for additional on-site storage. Use of this technology has expanded significantly since then, and has today become a standard part of plant operations at most US nuclear sites. As this expansion was underway, Federal programs remained stalled, and it became evident that dry cask systems would be in use longer than originally envisioned. In response to this challenge, a strong technical basis supporting the long term dry storage safety has been developed. However, this is not a static situation. The technical basis must be able to address future challenges. Industry is responding to one such challenge - the increasing prevalence of high burnup (HBU) used fuel and the need to provide long term storage assurance for these fuels equivalent to that which has existed for lower burnup fuels over the past 25 years. This response includes a confirmatory demonstration program designed to address the aging characteristics of HBU fuel and set a precedent for a learning approach to aging management that will have broad applicability across the used fuel storage landscape. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2015

System impacts of accelerated transfer of used nuclear fuel to dry storage - 15220

In the wake of the September 11, 2001 terror attacks, and again after the March 11, 2011, accident at the Fukushima Dai-Ichi station from the Great East Japan Earthquake/tsunami, concern was expressed regarding security of current spent fuel storage practices in the United States. An approach recurrently proposed to reduce the potential for fire and the release of radionuclides in an accident or sabotage scenario is to reduce the loading of the reactor fuel pools, which are frequently maintained near their full capacity at many reactor sites in the U.S. We assess the impact on the waste management system of different scenarios for accelerating the schedule of used nuclear fuel (UNF) transfer from reactor pools to dry storage casks. We consider scenarios where the spent fuel pools are drawn down to 50% or 25% of full capacity over 5- or 10-year schedules. The scenarios include status quo, where UNF continues to remain in dry storage at the reactor sites, as well as scenarios with UNF transfer to interim storage and eventually to a mined geologic repository. The primary purpose is to evaluate how the different scenarios for accelerating the transfer of UNF to at-reactor dry storage would affect the performance of the entire UNF management system. Areas that were considered include an estimate of the additional system costs that could be incurred and where the existing infrastructure at the reactor sites would come under stress from the transfer demands. This study considered only the fuel-handling logistics and rough-order-of-magnitude cost at reactor sites, interim storage facility, and operations to package UNF into disposal canisters. The effects of minimum fuel age that could be transferred and the accelerated transfer starting date are also examined, but found to have relatively little effect. Impacts on safety and worker dose are not evaluated quantitatively, although effects can be inferred from increases in handling operations, etc. from the scenarios considered. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗