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DOE OSTI2022

Photovoltaic windows cut energy use and CO 2 emissions by 40% in highly glazed buildings

Buildings account for 30% of global energy use. The architectural trend across building sectors is toward more glass despite higher energy use and carbon emissions than opaque cladding alternatives. Numerous window technologies - low-emissivity coatings, triple glazing, dynamic tinting, and the more recently developed photovoltaic glass - have emerged in the last two decades as approaches to reduce building energy. However, a comprehensive understanding of where and how these window technologies can be installed to enable optimal energy savings under different climate conditions remains limited. Here we test window technologies using thousands of macroscale building-energy simulations for different climate zones and building designs to evaluate the associated net energy use and carbon-emissions reduction potential. Novel window technologies, especially photovoltaic windows with high thermal performance, offer energy savings in all climates, ranging from 10,000-40,000 GJ per year over substandard windows for a typical office building, resulting in up to 2,000 tons of annual CO 2 emissions reduction. Highly glazed, net-zero buildings are achievable via photovoltaic windows when combined with careful geometric considerations.

14 SOLAR ENERGY↗

DOE OSTI2021

Additive manufacturing of cobalt-based alloy on tool steel by directed energy deposition

Cladding hard-surfacing alloys on tool steel is an effective approach to enhance the surface properties of tool steel. In this study, a Co-based alloy was deposited on tool steel by Directed Energy Deposition (DED) following a three-factor three-level design of experiment matrix with varied laser power, scan speed, and powder flow rate. The microstructure of the deposits was characterized using scanning electron microscopy (SEM). The residual stress on the surface of the samples was measured by the X-ray diffraction (XRD) sin2? technique. The parameters that produced promising deposits were used to fabricate samples for tensile test, four-point bending test, Charpy impact test, and hardness measurement. Our result reveals that the processing parameters have a significant role in the residual stress of the coatings. Residual stress reduces with the increase of laser energy density. Cracks were found at samples with energy density below a threshold. Tensile testing of the coating/substrate combined structure reveals fracture at the coatings with an ultimate tensile strength of 633.9 ± 54.7 MPa. The bi-material interface survived the tensile test, indicating a strong interfacial bond. The four-point bending test of coating/substrate laminates shows an ultimate flexure strength of 860.6 ± 36.9 MPa. Cracks initiated from the coatings ignored the interface and penetrated the substrate, suggesting a solid bi-material bond. Charpy impact test shows the absorbed energy of coating/substrate laminates is more than doubled that of the substrate.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Preliminary conceptual design of fast neutron spectrum nuclear thermal rocket cores using monolithic uranium nitride fuel

This paper presents a few nuclear thermal rocket (NTR) reactor core preliminary conceptual designs based on the use of monolithic uranium nitride (UN) fuel plates or pins clad with tungsten (W), alloyed or unalloyed as needed. High-assay low-enriched uranium (HALEU) as well as high-enriched uranium (HEU) are considered. Nominal core thermal powers are between 300 and 1100 MW corresponding to thrusts between 66 kN and 240 kN. The estimated thrust-to-reactor-weight ratios (T/WRx) achievable with the HEU plate and pin configurations are between 3.8 and 10.9. The T/WRx achievable with the HALEU plate and pin configurations are lower, 1.9–4.0, than those achievable with HEU. It is noteworthy that even a relatively modest increase in fuel enrichment above the HALEU limit enables a significant increase in T/WRx. It must be emphasized that these results do not yet account for uncertainties and that the appropriateness of the assumed fuel thermal design limits for normal operation (i.e., peak centerline temperature of 3100 K) will need to be confirmed. Finally, just like for the other UN-based fuels currently considered for NTR applications (i.e., CERMET and CERCER), the proposed UN fuel systems need significant testing in prototypic conditions to confirm the appropriate performance for safe NTR applications. However, the monolithic fuel systems may have, overall, a higher technology readiness level (TRL), and, consequently, shorter fuel development and validation time may result.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2022

Prospects for additive manufacturing of nuclear fuel forms

Additive manufacturing (AM) is viewed as a critical enabling technology for achieving superior performance and improved economics across many sectors. Although the past decade has seen increased application of AM methods to nuclear reactor cladding and structural materials, exploration of AM as applied to the uranium-bearing nuclear fuel forms has been limited. The two major families of nuclear fuel forms (monolithic, particle/dispersion) are utilized with their own set of core objectives in mind, and their differences require distinct fabrication infrastructures. These reference fabrication methods impose many limitations on nuclear fuels. Further, both currently operating reactors and future concepts have the potential for improved performance if these accepted limitations are relaxed or removed entirely. The primary limitations of reference fabrication processes for the common nuclear fuel forms are outlined in this paper. This groundwork is then used to identify avenues of fuel performance specific to each of these fuel architectures that could be exploited if the restrictions of conventional fuel fabrication are removed. Moreover, multiple targets for AM studies are laid out for each of the major nuclear fuel variants. Finally, key strategic components to guide research activities in AM of nuclear fuels are outlined, with an emphasis on use of modeling and simulation to motivate research aims and embrace of an accelerated testing methodology to screen and quality new fuel forms.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2020

Particulate plutonium released from the Fukushima Daiichi meltdowns

Traces of Pu have been detected in material released from the Fukushima Daiichi Nuclear Power Plant (FDNPP) in March of 2011; however, to date the physical and chemical form of the Pu have remained unknown. Here we report the discovery of particulate Pu associated with cesium-rich microparticles (CsMPs) that formed in and were released from the reactors during the FDNPP meltdowns. The Cs-pollucite-based CsMP contained discrete U(IV)O 2 nanoparticles, <~10 nm, one of which is enriched in Pu adjacent to fragments of Zr-cladding. The isotope ratios, 235 U/ 238 U, 240 Pu/ 239 Pu, and 242 Pu/ 239 Pu, of the CsMPs were determined to be ~0.0193, ~0.347, and ~0.065, respectively, which are consistent with the calculated isotopic ratios of irradiated-fuel fragments. Thus, considering the regional distribution of CsMPs, the long-distance dispersion of Pu from FNDPP is attributed to the transport by CsMPs that have incorporated nanoscale fuel fragments prior to their dispersion up to 230 km away from the Fukushima Daiichi reactor site.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

DOE OSTI2022

Deformation mechanism in nanolaminate FeCrAl alloys by ,em>in situ micromechanical strain rate jump tests at elevated temperatures

FeCrAl alloys have attracted extensive attention as one of the potential cladding materials for the commercial light water reactors. Although the creep behaviors of coarse-grain FeCrAl alloys have been investigated at elevated temperatures, little is known on the deformation mechanism of fine-grain FeCrAl alloys. We performed surface mechanical grinding treatment to fabricate nanolaminated ferritic FeCrAl alloys. In situ micropillar compression tests were applied to determine the underlying deformation mechanism of nanolaminated FeCrAl alloys at elevated temperatures. The strain rate sensitivity and activation energy for the dominant deformation mechanism were estimated considering the presence of a threshold stress.

36 MATERIALS SCIENCE↗

DOE OSTI2026

In-situ synchrotron X-ray investigation of phase evolution in gas atomized powder enabling manufacturing of nanoscale oxide-dispersion strengthened ferritic steels

Here, we present an investigation of Fe-14Cr-3W-0.4Y-0.4Zr-0.18Ti (wt.%) as a reduced-activation oxide-dispersion strengthened (ODS) ferritic steel, an alternative to the “14YWT” structural alloys designed for nuclear energy applications. Gas atomization reaction synthesis (GARS) was used to produce these Zr-modified powders with a non-equilibrium (metastable) phase that enable a heat treatment (delayed) route for producing nanoscale oxide-dispersion strengthening. In situ synchrotron X-ray diffraction and transmission electron microscopy were used to analyze phase evolution as a function of temperature and time, revealing formation of highly dispersed oxide nanoprecipitate phases at temperatures above those needed for powder consolidation and shaping of components. This would allow fabrication of net-shape parts using conventional powder-processing methods prior to thermal activation of a reaction producing nanocrystalline Y-(Ti, Zr)-O particles, with a size of 20 ± 7 nm. These results can inform processing of tubes, cladding, sheets, and plates for use in advanced fission and fusion reactors.

In-situ synchrotron X-ray diffraction↗

DOE OSTI2020

Single Entity Electrochemistry in Nanopore Electrode Arrays: Ion Transport Meets Electron Transfer in Confined Geometries

Electrochemical measurements conducted in confined volumes provide a powerful and direct means to address scientific questions at the nexus of nanoscience, biotechnology, and chemical analysis. How are electron transfer and ion transport coupled in confined volumes and how does understanding them require moving beyond macroscopic theories? Also, how do these coupled processes impact electrochemical detection and processing? We address these questions by studying a special type of confined-volume architecture, the nanopore electrode array, or NEA, which is designed to be commensurate in size with physical scaling lengths, such as the Debye length, a concordance that offers performance characteristics not available in larger scale structures. The experiments described here depend critically on carefully constructed nanoscale architectures that can usefully control molecular transport and electrochemical reactivity. We begin by considering the experimental constraints that guide the design and fabrication of zero-dimensional nanopore arrays with multiple embedded electrodes. These zero-dimensional structures are nearly ideal for exploring how permselectivity and unscreened ion migration can be combined to amplify signals and improve selectivity by enabling highly efficient redox cycling. Our studies also highlight the benefits of arrays, in that molecules escaping from a single nanopore are efficiently captured by neighboring pores and returned to the population of active redox species being measured, benefits that arise from coupling ion accumulation and migration. These tools for manipulating redox species are well-positioned to explore single molecule and single particle electron transfer events through spectroelectrochemistry, studies which are enabled by the electrochemical zero-mode waveguide (ZMW), a special hybrid nanophotonic/nanoelectronic architecture in which the lower ring electrode of an NEA nanopore functions both as a working electrode to initiate electron transfer reactions and as the optical cladding layer of a ZMW. Furthermore, while the work described here is largely exploratory and fundamental, we believe that the development of NEAs will enable important applications that emerge directly from the unique coupled transport and electron-transfer capabilities of NEAs, including in situ molecular separation and detection with external stimuli, redox-based electrochemical rectification in individually encapsulated nanopores, and coupled sorters and analyzers for nanoparticles.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

422 Million intrinsic quality factor planar integrated all-waveguide resonator with sub-MHz linewidth

High quality-factor (Q) optical resonators are a key component for ultra-narrow linewidth lasers, frequency stabilization, precision spectroscopy and quantum applications. Integration in a photonic waveguide platform is key to reducing cost, size, power and sensitivity to environmental disturbances. However, to date, the Q of all-waveguide resonators has been relegated to below 260 Million. Here, we report a Si 3 N 4 resonator with 422 Million intrinsic and 3.4 Billion absorption-limited Qs. The resonator has 453 kHz intrinsic, 906 kHz loaded, and 57 kHz absorption-limited linewidths and the corresponding 0.060 dB m -1 loss is the lowest reported to date for waveguides with deposited oxide upper cladding. These results are achieved through a careful reduction of scattering and absorption losses that we simulate, quantify and correlate to measurements. This advancement in waveguide resonator technology paves the way to all-waveguide Billion Q cavities for applications including nonlinear optics, atomic clocks, quantum photonics and high-capacity fiber communications.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Bidirectional interconversion of microwave and light with thin-film lithium niobate

Abstract Superconducting cavity electro-optics presents a promising route to coherently convert microwave and optical photons and distribute quantum entanglement between superconducting circuits over long-distance. Strong Pockels nonlinearity and high-performance optical cavity are the prerequisites for high conversion efficiency. Thin-film lithium niobate (TFLN) offers these desired characteristics. Despite significant recent progresses, only unidirectional conversion with efficiencies on the order of 10 −5 has been realized. In this article, we demonstrate the bidirectional electro-optic conversion in TFLN-superconductor hybrid system, with conversion efficiency improved by more than three orders of magnitude. Our air-clad device architecture boosts the sustainable intracavity pump power at cryogenic temperatures by suppressing the prominent photorefractive effect that limits cryogenic performance of TFLN, and reaches an efficiency of 1.02% (internal efficiency of 15.2%). This work firmly establishes the TFLN-superconductor hybrid EO system as a highly competitive transduction platform for future quantum network applications.

42 ENGINEERING↗

DOE OSTI2023

Investigations towards incorporation of Eu 3+ and Cm 3+ during ZrO 2 crystallization in aqueous solution

Nuclear energy provides a widely applied carbon-reduced energy source. Following operation, the spent nuclear fuel (SNF), containing a mixture of radiotoxic elements such as transuranics, needs to be safely disposed of. Safe storage of SNF in a deep geological repository (DGR) relies on multiple engineered and natural retention barriers to prevent environmental contamination. In this context, zirconia (ZrO 2 ) formed on the SNF rod cladding, could be employed as an engineered barrier for immobilization of radionuclides via structural incorporation. This study investigates the incorporation of Eu 3+ and Cm 3+ , representatives for trivalent transuranics, into zirconia by co-precipitation and crystallization in aqueous solution at 80 °C. Complementary structural and microstructural characterization has been carried out by powder X-ray diffraction (PXRD), spectrum imaging analysis based on energy-dispersive X-ray spectroscopy in scanning transmission electron microscopy mode (STEM-EDXS), and luminescence spectroscopy. The results reveal the association of the dopants with the zirconia particles and elucidate the presence of distinct bulk and superficially incorporated species. Hydrothermal aging for up to 460 days in alkaline media points to great stability of these incorporated species after initial crystallization, with no indication of phase segregation or release of Eu 3+ and Cm 3+ over time. These results suggest that zirconia would be a suitable technical retention barrier for mobilized trivalent actinides in a DGR.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2025

Tensile properties of the neutron irradiated HT-9 ACO-3 duct

HT-9, a ferritic-Martensitic steel, has attracted significant interest as a structural and cladding material for a variety of high dose nuclear component applications. This study examines the tensile properties of a HT-9 fuel assembly duct from the fast flux test facility, FFTF. The duct, from the Advanced Core Oxide-3 (ACO-3) irradiation test, was subjected to fast neutron irradiation exposure ranging from 3 dpa above the core top to nearly 155 dpa near the core mid-plane, spanning a temperature range from 382 °C at the lower end to 504 °C at the top. Due to the combination of thermal and neutron flux gradients along the core height. This yields a variety of irradiation damage processes which depend on core location. Tensile properties of specimens extracted at different positions along the height of the irradiated duct were measured at 25 °C, 200 °C and near their in-core irradiation temperature. The results show temperature has a greater impact than dose on post-irradiation strength and ductility. Two irradiation temperature regimes were determined, below irradiation temperatures of 420 °C irradiation hardening increases as irradiation temperature decreases, and above that temperature relatively minor changes are observed in tensile properties. These results are discussed in terms of expected microstructural changes, indicating that dislocation content is a strong contributor in these findings.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2021

Safely probing the chemistry of Chernobyl nuclear fuel using micro-focus X-ray analysis

Detailed chemical analysis of the solidified molten fuel still residing in the stricken Chernobyl reactor unit 4 are inferred using multi-modal micro-focus X-ray analysis of a low-radioactivity proxy. A fascinating mixture of molten UO 2 , nuclear fuel cladding, concrete, stainless steel and other nuclear reactor components, these materials behaved like lava, solidifying to form a complex, highly radioactive glass-ceramic. Using element-specific chemical probes (micro-X-ray fluorescence and X-ray absorption spectroscopy), coupled with micro-diffraction analysis, the crystalline phase assemblage of simulants of these heterogeneous materials was established, which included “chernobylite” and a range of compositions in the (U 1-x Zr x )O 2 solid solution. Novel insight to nuclear accident fuel chemistry was obtained by establishing the oxidation state and local coordination of uranium not only in these crystalline phases, but uniquely in the amorphous fraction of the material, which varied depending on the history of the nuclear lava as it flowed through the reactor. This study demonstrates that micro-focus X-ray analysis of very small fractions of material can yield rich chemical information, which can be applied to nuclear-melt down materials to aid decommissioning and nuclear fuel management at nuclear accident sites.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2020

An Improved Energy Deposition Model in MPACT and Explicit Heat Generation Coupling with CTF

The default energy deposition model in the CASL neutronics code MPACT assumes all fission energy is deposited locally in fuel rods. Furthermore, equilibrium delayed energy release is assumed for both steady-state and transient calculations. These approximations limit the accurate representation of the heat generation distribution in space and its variations over time, which are essential for power distribution and thermal-hydraulic coupling calculations. In this paper, an improved energy deposition model is presented in both the spatial and time domains. Spatially, the energy deposition through fission, neutron capture, and slowing-down reactions are explicitly modeled to account for the heat generation from all regions of a reactor core, and a gamma smearing scheme is developed that utilizes the gamma sources from neutron fission and capture. In the time domain, the delayed energy release is modeled by solving an additional equation of delayed heat emitters, similar to the equation of delayed neutron precursors.To allow the explicit heat generation coupling, the interfaces between MPACT and CTF were updated to transfer separate heat sources for different material regions (fuel, clad, moderator and guide tube). The results show that the distributions of the energy deposition between MPACT and MCNP agree very well for various 2-D assembly and quarter-core problems without TH feedback. The MPACT/CTF coupled calculation for the hot full power quarter-core case exhibited a reduced peak pin power by 2.3% and a reduced peak fuel centerline temperature by 17 K when using the explicit energy deposition and heat transfer. The new model also shows a maximum 100 pcm keff effect on assembly depletion problems and an increased overall energy release by 7% in a PWR reactivity-initiated accident (RIA) problem.

Liu, Yuxuan↗

DOE OSTI2020

Intrinsic thermal interfacial resistance measurement in bonded metal–polymer foils

Heat conduction through bonded metal–polymer interfaces often limits the overall heat transfer in electronic packaging, batteries, and heat recovery systems. To design the thermal circuit in such systems, it is essential to measure the thermal interfacial resistance (TIR) across ~1 µm to 100 µm junctions. Previously reported TIR of metal–polymer junctions utilize ASTM E1530-based two-block systems that measure the TIR by applying pressure across the interface through external heating and cooling blocks. Here, we report a novel modification of the ASTM-E1530 technique that employs integrated heaters and sensors to provide an intrinsic TIR measurement of an adhesively bonded metal–polymer junction. We design the measurement technique using finite element simulations to either passively suppress or actively compensate the lateral heat diffusion through the polymer, which can minimize the systematic error to ≲5%. Through proof-of-concept experiments, we report the TIR of metal–polymer interfaces made from DuPont’s Pyralux double-side copper-clad laminates, commonly used in flexible printed circuit boards. Our TIR measurement errors are <10%. We highlight additional sources of errors due to non-idealities in the experiment and discuss possible ways to overcome them. Our measurement technique is also applicable to interfaces that are electrically insulating such as adhesively joined metal–metal junctions and sputter-coated or welded metal–polymer junctions. Altogether, the technique is capable of measuring TIR ≳10 –5 m 2 KW –1 in bonded metal–polymer foils and can be tailored for in situ measurements in flexible electronics, circuit packaging, and other hybrid metal–polymer systems.

47 OTHER INSTRUMENTATION↗

DOE OSTI2022

Multifunctional nanopore electrode array method for characterizing and manipulating single entities in attoliter-volume enclosures

Structurally regular nanopore arrays fabricated to contain independently controllable annular electrodes represent a new kind of architecture capable of electrochemically addressing small collections of matter—down to the single entity (molecule, particle, and biological cell) level. Furthermore, these nanopore electrode arrays (NEAs) can also be interrogated optically to achieve single entity spectroelectrochemistry. Larger entities such as nanoparticles and single bacterial cells are investigated by dark-field scattering and potential-controlled single-cell luminescence experiments, respectively, while NEA-confined molecules are probed by single molecule luminescence. By carrying out these experiments in arrays of identically constructed nanopores, massively parallel collections of single entities can be investigated simultaneously. The multilayer metal–insulator design of the NEAs enables highly efficient redox cycling experiments with large increases in analytical sensitivity for chemical sensing applications. NEAs may also be augmented with an additional orthogonally designed nanopore layer, such as a structured block copolymer, to achieve hierarchically organized multilayer structures with multiple stimulus-responsive transport control mechanisms. Finally, NEAs constructed with a transparent bottom layer permit optical access to the interior of the nanopore, which can result in the cutoff of far-field mode propagation, effectively trapping radiation in an ultrasmall volume inside the nanopore. Furthermore, the bottom metal layer may be used as both a working electrode and an optical cladding layer, thus, producing bifunctional electrochemical zero-mode waveguide architectures capable of carrying out spectroelectrochemical investigations down to the single molecule level.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

The Complex, Unique, and Powerful Imaging Instrument for Dynamics (CUPI 2 D) at the Spallation Neutron Source (invited)

The Oak Ridge National Laboratory is planning to build the Second Target Station (STS) at the Spallation Neutron Source (SNS). STS will host a suite of novel instruments that complement the First Target Station’s beamline capabilities by offering an increased flux for cold neutrons and a broader wavelength bandwidth. A novel neutron imaging beamline, named the Complex, Unique, and Powerful Imaging Instrument for Dynamics (CUPI 2 D), is among the first eight instruments that will be commissioned at STS as part of the construction project. CUPI 2 D is designed for a broad range of neutron imaging scientific applications, such as energy storage and conversion (batteries and fuel cells), materials science and engineering (additive manufacturing, superalloys, and archaeometry), nuclear materials (novel cladding materials, nuclear fuel, and moderators), cementitious materials, biology/medical/dental applications (regenerative medicine and cancer), and life sciences (plant–soil interactions and nutrient dynamics). The innovation of this instrument lies in the utilization of a high flux of wavelength-separated cold neutrons to perform real time in situ neutron grating interferometry and Bragg edge imaging—with a wavelength resolution of δλ/λ ≈ 0.3%—simultaneously when required, across a broad range of length and time scales. This manuscript briefly describes the science enabled at CUPI 2 D based on its unique capabilities. The preliminary beamline performance, a design concept, and future development requirements are also presented.

47 OTHER INSTRUMENTATION↗

DOE OSTI2023

Continuous wave room temperature operation of the 2 $μ$m GaSb-based photonic crystal surface emitting diode lasers

Continuous wave room temperature operation of 2 μm GaSb-based photonic-crystal surface-emitting diode lasers has been realized. The deep etched square mesa devices showed threshold current densities of 500 A/cm 2 at 20 °C. The epi-side down mounted lasers generated above 10 mW of output power in the continuous wave regime and tens of milliwatts in pulses from the 200 × 200 μm 2 aperture. Here, the breakthrough in the device performance parameters was achieved thanks to a highly homogeneous air-pocket retaining epitaxial regrowth process optimized for a specifically designed antimonide diode laser heterostructure. The nanofabrication method utilizing low temperature atomic hydrogen surface cleaning yielded low disorder square lattice of droplet-shaped voids covered by uniform p-cladding layer. The laser emission spectrum as well as near/far field patterns demonstrated peculiar features presumably linked to deformation of the void shape during regrowth and formation of the array of filaments.

77 NANOSCIENCE AND NANOTECHNOLOGY↗