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At least 163 records · Page 9

Understanding the Structure and Dynamics of Conjugated Polymers by Advancing Deuteration Chemistry and Neutron Scattering (Final Report)

The overarching goal of the proposed work was to set up a partnership between the University of Southern Mississippi (USM) and Oak Ridge National Laboratory (ORNL) to develop novel approaches to measure the backbone rigidity of conjugated polymers (CPs) and understand the critical role of sidechains on the backbone conformation and the materials macroscopic property. The backbone rigidity greatly influences the electronic properties of CPs, which ultimately determines the functionality and performance of these materials. Improvements in the electronic properties of CPs would allow for enhanced charge transport in semiconductor devices, improved photovoltaic performance, recycling of waste heat in thermoelectrics, and discovery of new phenomena that will enable the next generation of energy technologies. Although significant progress has been made to optimize the optical and electronic properties of CPs, largely through Edisonian methodologies, it remains a challenge to experimentally characterize conjugated backbone conformation (chain rigidity, torsion, planarity, and short-range order) and relate these to the fundamental optical and electronic properties (electronic coupling, charge transport, etc.). This has left fundamental gaps in our knowledge of the most basic structure/property relationships within these systems, precluded the study of fundamental physical phenomena, and constrained the design and realization of new electronic and device functionalities. Thus, the major goal of this work is to use novel deuteration methodologies via systematic synthetic approaches, and neutron scattering techniques to comprehensively characterize the structural and dynamic properties of CPs in contrast-matching solvents. Our work would, for the first time, elucidate the relationship between backbone rigidity and macroscopic properties. They will also allow a rational formulation of design principles for next-generation CPs that are resilient to disorder through precise control of the delocalized electrons along the polymer backbone. Overall, this project will advance our understanding of the structure, dynamics, and fundamental physics of these materials, which is crucial for enabling the prediction, design, control, and manipulation of current and emerging material electronic properties.

36 MATERIALS SCIENCE↗

Analysis Of The Sludge Batch 7b (Macrobatch 9) DWPF Pour Stream Glass Sample (Rev. 1)

The Defense Waste Processing Facility (DWPF) began processing Sludge Batch 7b (SB7b), also referred to as Macrobatch 9 (MB9), in January 2012. SB7b is a blend of the heel of Tank 40 from Sludge Batch 7a (SB7a) and the SB7b material that was transferred to Tank 40 from Tank 51. SB7b was processed using Frit 418. During processing of each sludge batch, the DWPF is required to take at least one glass sample to meet the objectives of the Glass Product Control Program (GPCP), which is governed by the DWPF Waste Form Compliance Plan, and to complete the necessary Production Records so that the final glass product may be disposed of at a Federal Repository. Two pour stream glass samples were collected while processing SB7b. The samples were transferred to the Savannah River National Laboratory (SRNL) where one was analyzed and the other was archived. The following conclusions were drawn from the analytical results provided in this report: The sum of oxides for the official SB7b pour stream glass is within the Product Composition Control System (PCCS) limits (95-105 wt%); The average calculated Waste Dilution Factor (WDF) for SB7b is 2.3. In general, the measured radionuclide content of the official SB7b pour stream glass is in good agreement with the calculated values from the Tank 40 dried sludge results from the SB7b Waste Acceptance Program Specification (WAPS) sample; As in previous pour stream samples, ruthenium and rhodium inclusions were detected by Scanning Electron Microscopy-Electron Dispersive Spectroscopy (SEM-EDS) in the SB7b pour stream sample; The Product Consistency Test (PCT) results indicate that the official SB7b pour stream glass meets the waste acceptance criteria for durability with a normalized boron release of 0.8 g/L, which is an order of magnitude less than the Environmental Assessment (EA) glass; The measured density of the SB7b pour stream glass was 2.70 g/cm 3 ; The Fe 2+ /ΣFe ratio of the SB7b pour stream samples was 0.07.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Broad Distribution of Local Polar States Generates Large Electrothermal Properties in Pb-Free Relaxor Ferroelectrics

Electrothermal energy conversion provides attractive solutions for global energy management, such as energy harvesting from waste heat using pyroelectric energy conversion (PEC) and efficient cooling of portable electronics or data servers using the electrocaloric effect. Relaxor ferroelectrics are attractive for electrothermal energy conversion because of their large pyroelectric coefficients over a wide temperature range. Although Pb-based relaxors are well-known, toxicity concerns have mandated the intense search for Pb-free alternatives. Here, we engineered (Ba,Ca)TiO 3 -based relaxors based on a multisite doping strategy, which show promising electrothermal performance, viz. a maximum PEC efficiency of 14% and electrocaloric refrigeration capacity of 115 J/kg. Using local-scale structural analysis, we provide an atomistic model for large electrothermal properties in the newly designed Pb-free ferroelectrics, whereby a temperature-independent continuous distribution of cation displacement directions creates easy pathways for microscopic polarization reorientation. This research provides key structural insight for future atomic-scale engineering of environmentally sustainable ferroelectrics in energy applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Bioenergy Feedstock Library Annual Summary Report

The Bioenergy Feedstock Library (BFL), part of the Biomass Feedstock National User Facility (BFNUF) located at INL, is a physical sample repository and a web-accessible electronic database. The BFL stores physical and chemical characteristics of biomass and waste carbon sources for energy use as well as samples generated from across U.S. Department of Energy (DOE) Bioenergy Technologies Office (BETO) funded projects. The objective of this Bioenergy Feedstock Library Annual Summary Report for 2022 is to focus on the (1) publicly available analytical data and equipment tracked through the BFNUF, (2) physical samples available for request, (3) sample and data archival progress from recent BETO-funded projects, and (4) publicly available data sets created upon request from BETO, INL projects, or outside entities. This report highlights key statistics from FY22 and available data and information important for INL, BFL users, academics, and industry.

09 BIOMASS FUELS↗

Bioenergy Feedstock Library 2023 Annual Summary Report

The Bioenergy Feedstock Library (BFL), part of the Biomass Feedstock National User Facility (BFNUF) located at INL, is a physical sample repository and a web-accessible electronic database. The BFL stores physical and chemical characteristics of biomass and waste carbon sources for energy use as well as samples generated from across U.S. Department of Energy (DOE) Bioenergy Technologies Office (BETO) and U.S. Department of Agriculture funded projects. The objective of this Bioenergy Feedstock Library Annual Summary Report for 2023 is to focus on the updates to (1) publicly available analytical data and equipment tracked through the BFNUF, (2) physical samples available for request, (3) sample and data archival progress from recent BETO-funded projects, and (4) publicly available datasets created upon request from BETO, INL projects, or outside entities compared to the 2022 Bioenergy Feedstock Library Annual Summary Report. This report highlights key statistics and available data and information important for INL, BFL users, academics, and industry.

09 BIOMASS FUELS↗

Bioenergy Feedstock Library Annual Summary Report 2024

The Bioenergy Feedstock Library (BFL), part of the Biomass Feedstock National User Facility (BFNUF) located at Idaho National Laboratory (INL), is a physical sample repository and a web-accessible electronic database. The BFL stores physical and chemical characteristics of biomass and waste carbon sources for energy use, as well as samples generated from U.S. Department of Energy (DOE) Bioenergy Technologies Office (BETO) and U.S. Department of Agriculture-funded projects. The objective of this Bioenergy Feedstock Library Annual Summary Report for 2024, similar to the 2023 Annual Summary Report , is to focus on the updates to: (1) publicly available analytical data and equipment tracked through the BFNUF, (2) significant increases in the physical samples available for request, (3) sample and data archival progress from recent BETO-funded projects, and (4) publicly available data sets created upon request from BETO, INL projects, or outside entities compared to the previous annual summary reports. This report highlights key statistics and available data and information important for INL, BFL users, academics, and industry.

09 BIOMASS FUELS↗

Heat pipe applications for the space shuttle.

Discussion of six specific applications for heat pipe (HP) devices on the space shuttle. These applications were chosen from 27 concepts formulated as part of a study to evaluate the potential benefits associated with HP use. The formulation process is briefly described along with the applications which evolved. The bulk of the discussion deals with the 'top' six - namely, HP radiators for waste heat rejection, an HP augmented cold rail, an HP circuit for electronic equipment cooling, modular heat sink for control of remote packages, an HP temperature control for compartments, and air-cooled equipment racks. The philosophy, physical design details, and performance data are presented for each concept along with a comparison with the baseline design where applicable.

Tawil, M.↗

First-principles calculation of lattice distortion, electronic structure, and bonding properties of GeTe-based and PbSe-based high-entropy chalcogenides

The massive amount of wasted heat energy from industry has pushed the development of thermoelectric (TE) materials that directly convert heat into electricity to a new level of concern. Recently, multicomponent alloys such as GeTe-based and PbSe-based high-entropy (HE) chalcogenides have attracted a great deal of attention due to their potential application as TE materials. The nature of the interatomic bonding, lattice distortion (LD), and the electronic structure in this class of materials is not fully understood. Herein, we report a comprehensive computational investigation of nine GeTe-based HE alloys with eight metallic elements (Ag, Pb, Sb, Bi, Cu, Cd, Mn, and Sn) with large supercells of 1080 atoms each; seven PbSe-based HE solid solutions: Pb0.99−ySb0.012SnySe1−2xTexSx (x = 0.1, 0.2, 0.25, 0.3, 0.35, 0.4, 0.45, with y = 0) with supercells of 1000 atoms each; and five Pb0.99−ySb0.012SnySe1−2xTexSx (y = 0.05, 0.1, 0.15, 0.2, 0.25 with x = 0.25) solid solutions with supercells of 1000 atoms each. All these HE models are theoretically investigated for the first time. The electronic structure, interatomic bonding, charge transfer, and lattice distortion (LD) are investigated by first-principles calculations based on density functional theory. Multicomponent HE alloys can cause a significant LD, which affects their mechanical, thermal, and TE properties. The calculations for the GeTe-based HE chalcogenides showed that they are semiconductors with a narrow bandgap, except for m8, which has a semi-metallic characteristic, and this makes them good candidates for TE applications. For most of these models, the Fermi level shifts upward and locates deeply in the conduction bands, resulting in the enhancement of the electrical conductivity (σ). The bonding properties showed that most bonds in m5 are more dispersed, indicating highest LD and lower lattice thermal conductivity. For PbSe-based HE solid solutions, the LD calculations showed that the models Pb0.99Sb0.012Se0.5Te0.25S0.25 and Pb0.89Sb0.012Sn0.1Se0.5Te0.25S0.25 have the higher LD, and thus a lower lattice thermal conductivity. Such investigations are in high demand since it enables us to design new HE chalcogenides for TE applications. We use the novel concept of total bond order density as a single quantum mechanical metric to characterize the internal cohesion of these HE alloys and correlate with calculated properties, especially the mechanical properties. This work provides a solid database for HE chalcogenides and a road map for many potential applications. Moreover, the computational procedure we developed can be used to design new HE chalcogenides for specific TE applications.

Physics↗

Modulating the Electronic Transport of 2D Sb2Te3 Nanoplates by Coinage Metal Intercalation

Thermoelectric materials are particularly relevant to the current energy infrastructure and demands of the 21st century, converting waste heat into usable electricity. The solution intercalation of zerovalent copper into Sb2Te3 nanoplates, a well-established thermoelectric material, is reported. The copper intercalant is homogeneously distributed throughout the nanoplates, confirmed by scanning transmission electron microscopy coupled with energy-dispersive X-ray spectroscopy. The copper composition was shown to be 6 at. % by X-ray photoelectron spectroscopy. Copper ordering within the van der Waals gaps of the nanoplates is confirmed by selected area electron diffraction. Fabrication and thermoelectric property measurements of single-crystal Sb2Te3 and Cu-Sb2Te3 nanoplate devices show effective modulation of electrical conductivity and Seebeck coefficient with Cu intercalation. X-ray photoelectron spectroscopic studies in the valence-band region reveal additional electronic states from copper that appear near the Fermi energy, postulated to act as electron acceptors, leading to modulation of the electronic transport properties.

2D nanoplates↗

Early-stage oxidation and subsequent damage of the used nuclear fuel extractant TODGA; electron pulse radiolysis and theoretical insights

Radiation induced damage of extractant molecules is a well-known phenomenon responsible for reducing efficiency and increasing the waste and cost of reprocessing used nuclear fuel (UNF). As such, understanding early-stage (pico- to nanoseconds) radiation-induced reaction mechanisms is essential for informing the design of next generation extractants with enhanced radiation robustness. Here, in this work, we utilized picosecond and nanosecond electron pulse radiolysis experiments to probe the early-stage radioactive environment experienced by the organic phase extractant N,N,N',N'-tetraoctyldiglycolamide (TODGA), proposed for separating highly radioactive trivalent minor actinides (specifically americium and curium) from the trivalent lanthanides. Using comparisons to the similar ionization potential (IP) solute p-xylene, this work determined the mechanism of reaction with the ionized diluent (i.e., n-dodecane radical cation, DD˙ + ) is hole transfer to produce TODGA˙ + . At high TODGA concentrations (>100 mM), the majority of this transfer occurs faster than 10 ps via the capture of DD˙ + holes prior to their solvation with a C 37 = 300 mM. The surviving solvated holes were captured with k = (2.38 ± 0.15) × 10 10 M -1 s -1 . Attempts at subsequent hole transfer to lower IP solutes found that only 10% of holes were transferred, indicating bond rupture of TODGA˙ + occurs within 2.6 ns at 200 mM TODGA. Possible reaction pathways for the rapid decomposition of TODGA˙ + were explored using a combination of experiments and density functional theory (DFT) calculations.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Controllable Multi-Functional Heat Exchanger for Space Applications

Team Spacering will design SpaceRing, a cooling and waste heat recycling system that addresses NASA’s interest for a cooling and power-generating unit in its prototype deep space habitat[1]. The merits of this system are as follows: - Controllable cooling is critical in maintaining a habitable environment and in the functionality of life support systems, powering electronics and other devices in a spacecraft. - Power is expensive to produce in a space environment. Converting wasted thermal energy into electricity will save energy and money for the space station. Space habitation is a highly complex endeavor. Consequently, the SpaceRing must adhere to additional constraints, which include: - Lack of natural fluid or gas convection due to micro-gravity environment - Limited range for heat source and cold sink temperature - Subject to high fluctuations of incoming thermal energy - Minimal weight due to the high cost of transporting items into space After consulting with NASA and experts in thermal studies, several design objectives were identified and are listed below in order of importance: - High cooling capacity - Reliable safety control and alert system - Maximization of energy generation from wasted heat - Optimization of cooling capability and power generation - Long operational life and minimization of maintenance In space, conventional cooling systems utilize passive heat pipe systems for small-scale heat rejection and pumped pipes with heat exchangers for large-scale heat rejection. Thermal power generation in space is mainly achieved by using thermoelectric material that produces electric energy from temperature differentials. We propose a design that combines cooling and thermoelectric power generation. Using a hot pipe connected to a heat source, a cold pipe connected to a radiator, a heat exchanger in contact with both pipes, and a pump in each pipe to move the fluid, we make an active cooling system. The thermoelectric material is inserted in the heat exchanger between the hot and cold pipes to extract energy from the maximum temperature difference coming from the two pipes. It also provides controllable cooling capacity through the use of the thermoelectric material as cooling modules. We have tested our system under target heat source and sink conditions and measured the temperatures and flow rates. Our preliminary results are promising, demonstrating the output of 25 Watts of power on average. We are in the process of running control tests to compare the heat transfer performance without the thermoelectric generators, which is vital in determining whether or not the generators introduce an unacceptable amount of thermal resistance. While some control tests have been run already, the results have been noisy. We have modified our testing environment and data acquisition methods to allow for simple comparison between the control test results and thermoelectric performance results. Lastly, we have modified the heat exchanger design slightly to include acrylic baffles. This will allow the heat to flow through the heat exchanger more efficiently. We have presented our preliminary results to NASA and will deliver the final product by the end of May 2014.

Lee Xiong↗

Prediction for Pressure Differential Across HEPA Filter Media Based on Media Characteristics and Particle Size Distribution

A new method for predicting the pressure drop across High Efficiency Particulate Air (HEPA) filter media is proposed based upon mass deposited onto the filter and known physical characteristics of the filter media. Detailed are the methods used in conjunction with current filter loading models to predict the pressure drop, as well as tests conducted to validate the methods. The benefit of a prediction model for practical use lies in the manufacturing and service life of nuclear grade HEPA filters. HEPA filters for use in nuclear facilities have a prescribed expiration date and a maximum allowable operating pressure drop. Therefore, the ability to predict the pressure drop across a filter and relate it to an expected length of service time can enable a reduction in wasted filters. This will allow for more informed decisions to be made based upon the dictated life cycle of the filters. Also, understanding and predicting how the pressure drop of HEPA filter media behaves as a function of physical characteristics and loaded mass can assist in future design and manufacturing of filter media. Currently, most existing pressure drop models are either computationally based or analytical methods relying on data gathered during tests. Neither are practical for prediction; the computational methods are difficult to implement, and the current analytical methods are more useful as tools for analysis. The current analytical model developed by Bergman et al. is based upon the pressure drop from each media fiber and modeling the deposited particles as newly formed fibers. Using Bergman's model and the media properties, air properties, and known aerosol particle size distribution, a pressure drop curve as a function of loaded mass can be created. This curve implies initial loading in the depth of the filter media with a transition to pure surface loading on the filter face, and a sensitivity to an evolving particle size distribution as mass continues to load onto the filter. To implement the predictive model, knowledge of the mean filter fiber diameter and porosity of the filter media is required. Traditionally, the mean fiber diameter is calculated as an effective diameter from prior media testing, however, in this study a Scanning Electron Microscope (SEM) technique is used to acquire this variable. Validation of the predictive model is provided by flat sheet media tests under a controlled environment with a measured particle size distribution of the challenge aerosol and shows reasonable preliminary agreement.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Irradiation Assessment of a Lightweight Industrial Robot - Towards Faster, Safer and Sooner Waste Decommissioning - 20317

Robotic systems have been successfully applied in the nuclear industry for several decades as a safe approach to minimize the exposure dose of human operators. As nuclear waste management and decommissioning gathers pace, there is an emerging interest integrating modern off-the-shelf industrial robots in nuclear robotic systems which make use of complex electronics and software to improve functionality over traditional machines. The use of the industrial robots will significantly increase the pace of development of automated waste management systems at a reduced cost, and although these off-the-shelf robots are proven robust in typical industrial environments, performance in radioactive environments is less clear. This paper investigates the performance degradation of a lightweight industrial robot (KUKA iiwa 7 LBR 800) in a controlled radiation field, aiming to simulate conditions in highly radioactive nuclear waste handling facilities. The degradation of the industrial robot's performance is identified while measuring the air kerma dose-tolerance of sensitive components, via a systematic experimental methodology. The experience from this experiment has demonstrated the significant capabilities of industrial robots, which tolerated a large gamma dose of 164 Gy before a system failure. Future tests are planned, aiming to enable faster, safer and sooner waste management and decommissioning using complex robotic systems. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

A Portable High-Density Power Technology for Space, Lunar, and Planetary Applications

A new direct energy conversion concept called Nuclear Thermionic Avalanche Cell (NTAC) combined with a Metallic Junction Thermoelectric (MJ-TE) generator, both invented and patented by NASA, offers high specific power for portable applications. Estimates based on experimental results suggest superior performance compared to radioisotope thermoelectric generators (RTG) by up to two orders of magnitude for the NTAC and three to four times better for the MJ-TE generator for the same mass. The NTAC technology can use a variety of radioisotopes including nuclear waste to liberate a large number of intra-band(IB), inner shell electrons of atoms (105 C/cm3) by gamma-ray photons (100 keV to MeV). In contrast, conventional power generation has poor specific power because they only utilize the valence band electrons (3C/cm3) of the semiconductor or free electrons (8×103 C/cm3) of the conductor.

NTAC↗

Novel waste-derived non-noble metal catalysts to accelerate acidic and alkaline hydrogen evolution reaction

Carbon substrate support is a promising approach to facilitate catalytic activity of non-noble metal catalysts in hydrogen evolution reactions (HER). Here, in this paper, we report a waste-derived electrocatalyst P-CoNiO 2 @NC synthesized under mild condition. It exhibits outstanding HER performance in both acid (η 10 = 64.6 mV) and alkaline (η 10 = 96.4 mV) condition with good stability. Especially, it begins to outperform commercial Pt/C when the current density is over 74 mA/cm 2 in acid electrolyte and 29 mA/cm 2 in alkaline electrolyte. Moreover, the waste-derived carbon substrate could effectively promote HER activity of other dual 3d TMOs such as Fe and Co, Fe and Ni. The improved HER activity originates from electron transfer, electronic structure adjustment and optimization of intermediates adsorption according to X -ray photoelectron spectroscopy and density functional theory calculations. This work provides a new insight for converting wastes into value-added products and a sustainable and friendly strategy to facilitate hydrogen energy production.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

From the Lab to your Sewage Plant – Accelerators for Environmental Applications

The history of environmental applications of ionizing irradiation dates back to the 80s and 90s of the last century. Electron beam has proven to be a useful tool for the treatment of industrial waste water and flue gases and is already in use in multiple pilot plants in East Europe and Asia. It also offers a new alternative for tackling rising challenges for the wastewater treatment industry of the future in form of newly discovered harmful contaminants. The talk presents developments that enable a technology transfer of well-established superconducting accelerator technology from science to this field of environmental applications with a focus on water treatment. Recent achievements and future concepts are summarized with an emphasis on the pioneering work done at Jefferson Lab.

Vennekate, Hannes↗

Power Conversion with a Stirling Cycle for Venus Surface Mission

The light-filtering characteristic of the dense, mostly-CO2 atmosphere of Venus, combined with the high atmospheric cloud cover, relegates the surface mission use of photovoltaic power systems and beckons for the independence and reliability of a nuclear-powered energy source. A multi-faceted Venus mission study was completed at NASA GRC in December of 2003 that resulted in the preliminary design of a helium- charged, kinematic Stirling converter, which is powered by nuclear, General Purpose Heat Source (GPHS) modules. The kinematic, Stirling power converter is configured to drive an electronics and sensor cooler in addition to a generator for electrical power. This paper briefly describes the design process and also describes and summarizes key features of the Stirling power converter preliminary design concept. With an estimated total efficiency of 23.4%, the power converter drives the electronics and sensor cooler, and also produces 100 watts of electricity. The converter rejects waste heat at a hot sink temperature of 500 C.

Mellott, Ken↗