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DOE OSTI2023

Integrated Quantum-Classical Protocol for the Realistic Description of Solvated Multinuclear Mixed-Valence Transition-Metal Complexes and Their Solvatochromic Properties

Linear cyanide-bridged polymetallic complexes, which undergo photoinduced metal-to-metal charge transfer, represent prototypical systems for studying long-range electron-transfer reactions and understanding the role played by specific solute–solvent interactions in modulating the excited-state dynamics. Here, to tackle this problem, while achieving a statistically meaningful description of the solvent and of its relaxation, one needs a computational approach capable of handling large polynuclear transition-metal complexes, both in their ground and excited states, as well as the ability to follow their dynamics in several environments up to nanosecond time scales. Here, we present a mixed quantum classical approach, which combines large-scale molecular dynamics (MD) simulations based on an accurate quantum mechanically derived force field (QMD-FF) and self-consistent QMD polarized point charges, with IR and UV–vis spectral calculations to model the solvation dynamics and optical properties of a cyano-bridged trinuclear mixed-valence compound (trans-[(NC) 5 Fe III (μ-CN)Ru II (pyridine) 4 (μ-NC)Fe III (CN) 5 ] 4– ). We demonstrate the reliability of the QMD-FF/MD approach in sampling the solute conformational space and capturing the local solute–solvent interactions by comparing the results with higher-level quantum mechanics/molecular mechanics (QM/MM) MD reference data. The IR spectra calculated along the classical MD trajectories in different solvents correctly predict the red shift of the CN stretching band in the aprotic medium (acetonitrile) and the subtle differences measured in water and methanol, respectively. By explicitly including the solvent molecules around the cyanide ligands and calculating the thermal averaged absorption spectra using time-dependent density functional theory calculations within the Tamm–Dancoff approximation, the experimental solvatochromic shift is quantitatively reproduced going from water to methanol, while it is overestimated for acetonitrile. This discrepancy can likely be traced back to the lack of important dispersion interactions between the solvent cyano groups and the pyridine substituents in our micro solvation model. The proposed protocol is applied to the ground state in water, methanol, and acetonitrile and can be flexibly generalized to study excited-state nonequilibrium solvation dynamics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Design and synthesis of diazirine‐containing dyes for polypropylene fibre: A study on the effect of alkyl chain

Abstract The dyeing of polypropylene fabrics utilising conventional‐disperse dyes often meets poor colour yield and fastness problems, fundamentally caused by the low affinity between dyes and polypropylene fibres. In this article, a new class of hydrophobic reactive dyes that can react with polypropylene were designed using diazirine moiety as a reactive group, azo structure as a chromophore, and an ester group as a linking bridge. The difference among these dyes was the alkyl chain length on the azo chromophore, which was used to fine‐tune the affinity between the dyes and fibre. The structures of the synthesised dyes and intermediates were characterised and confirmed using nuclear magnetic resonance, mass spectrometry, and infrared spectrometry. The absorption and thermal properties of the dyes were also studied to ensure their feasibility for dyeing application. In addition, the diazirine dyes were successfully applied to dye polypropylene fabrics using a two‐step process by dyeing in a non‐aqueous solvent and fixing it under heating. The dyes and polypropylene fibre were demonstrated to react, where the fixation values were in the range 64.5–76.4%. The systematic study of the structure–property relationship demonstrated the positive effect of the alkyl chain in promoting colour yield, however, accompanied by a slightly reduced fixation value. Due to the chemical bonding of the dye molecules to the fibre, the dyed polypropylene fabrics exhibited excellent colour fastness property, making the dyeing technology very promising for future industrial applications.

Guo, Guangluo↗

DOE OSTI2022

Review of Direct Neutron Conversion and Detection Processes

Commercial and laboratory neutron detection systems use indirect neutron response of materials like pressurized helium-3 (via nuclear reaction 3He(n, p)3H) to measure and count neutrons emanating from a source. Recently a host of semiconductors, especially a ternary semiconductor of lithium indium diselenide (6LiInSe2) and a quaternary alloy of enriched lithium-6, indium, phosphorous, and selenium (6LiInP2Se6), have shown promising neutron counting possibilities by directly converting neutrons into charge-carrying elements within the body of the semiconductor. These semiconductors have high thermal neutron capture cross sections, suitable energy bandgaps (~2.0 electron volts) for room-temperature operations, and a favorable electronic band structure for efficient electron charge transport. The article examines the semiconductor properties of these compounds in terms of their neutron counting capabilities and possible ways to extract neutron energy information from them. Lithium-6 and boron-10 (with thermal neutron absorption cross sections of 938 ± 6 and 3855 ± 26 barns, respectively) produce charged particles to be measured via indirect neutron interactions. The efficiency of indirect conversion neutron detectors is limited because of the inefficiencies in conversion mechanism. In case of direct conversion, the neutrons create charged particles in a single material for neutron capture and charge collection, increasing detection efficiency. Unlike 3He proportional counters, which provide no neutron energy information, the semiconductors can be used as neutron energy spectrometer. Fully resolved neutron energy by 6LiInP2Se6 from a plutonium-beryllium source has been reported in the literature. We will discuss the influence of these multilayered semiconductors’ crystallographic structures and growth techniques on neutron energy determination.

61 RADIATION PROTECTION AND DOSIMETRY↗

DOE OSTI2021

Theoretical Yields for 188 W Production in the High Flux Isotope Reactor

Accurately predicting the production yield of 188 W and 191 Os from enriched 186W metal rings irradiated in HFIR is not straightforward. Two key factors can lead to significant uncertainty or inaccuracy in yield predictions: The effect of neutron flux depression in the dense tungsten metal target. Inaccuracy of the currently published 187 W thermal neutron absorption cross section. This manuscript reports the calculated yields for 188 W, 191 Os, and total osmium mass for the NM-888 target that was irradiated in High Flux Isotope Reactor (HFIR) Cycles 487 and 488. Three different yield calculation methods were used and are described herein. The results are presented in terms of total yield and in terms of yield per target mass. This allows for an approximate estimation of yields for future targets of varying mass loading but with similar irradiation profiles. For more accurate prediction yields, target-specific models that account for target loading, target positioning within HFIR, and accurate HFIR cycle data are required.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2024

First-Principles Studies of Tritium Species Diffusivity Across the Interface of Nickel-Plated Zircaloy-4

α-Zr and its alloys are known as best 3 H getters due to their excellent corrosion resistance under chemically corrosive environment, low thermal neutron absorption cross-section and robust mechanical strength at high temperature. In this work, we conducted a systematic study on constructing and optimizing Ni and Zr surfaces, interfacing the stable Ni and Zr surfaces to create an optimal Ni-Zr interface, and an understanding the diffusion mechanisms for 3 H across Ni(111)-Zr(0001) interface with and without vacancies and impurities such as Sn and O.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2023

Modeling Advanced Strippers for CO2 Capture from Gas-Fired Power Plants using Aqueous Piperazine

Energy performance of 5 m piperazine was evaluated with an advanced stripper at the pilot scale, accounting for heat loss. Modeling studies indicated that heat loss at locations other than the heat source impacted the heat duty. For strippers with excess packing, the column was the most important source of heat loss, and values as low as 0.03 GJ/hr can cause pinch and reabsorption of CO2. Solvents like 5 m PZ are more affected by heat loss in the column due to a top-side temperature pinch at high lean loading. Heat loss impacts NGCC CO2 capture more than coal-based CO2 capture. Surface temperature measurements pilot plants showed that heat loss was 50-75% controlled by natural convection. Measured heat loss was correlated with steam flowrate and wind speed and ranged from 8126 to 219668 Btu/hr, representing 35% of the measured heat rate on average. Net heat duty linearly varied with CO2 removal at low lean loading and was similar for coal and NGCC conditions at fixed removal. At 90% removal, net heat duty was about 2.5 GJ/t with 4 and 12% CO2 in the flue gas. 7 At NGCC conditions, strippers with finite packing can benefit from a flashing feed to the top of the column by using a hot bypass. A flashing feed was linked to a reduction in irreversibility of the stripper from temperature driving forces. It also reduces heat duty by up to 6% at fixed packing height and reduces packing requirement for a fixed steam heater size compared to a warm bypass. Lean loading and lean solvent rate were effective handles to maximize profitability of a fixed stripper design at low gas price. High ambient temperature operation can benefit from low pressure stripping to about 0.18 lean loading at 150 ℃ to maintain the cyclic capacity at reduced rich loading. At low gas price, the capture plant was able to maximize profitability even with a high heat duty of 2.7-3.1 GJ/t at a lean loading of 0.2-0.22 mol/mol. Heat recovery by partial water vapor condensation in a gas-liquid exchanger can be replaced by a direct contact condenser (DCC). The DCC improved gas cooling and reduced heat duty compared to the CO2 exchanger at 0.2 lean loading. The DCC when used with a 150 ℃/5.5 bar stripper can reduce the cost of capture compared to the base case by $3- 4/tonne at 15 ft of packing (optimum) but increases cost of capture by $6/tonne with a 120 ℃/2 bar stripper and 10 ft of packing (optimum). The DCC can work effectively with a solvent with a high heat of absorption and thermal stability.

Suresh Babu, Athreya↗

DOE OSTI2024

Fractal Nanostructured Solar Selective Surfaces for Next Gen Concentrating Solar Power (Final Report)

This project reports a novel coating with enhanced solar absorptance and reduced thermal emittance with high efficiency at elevated temperature for next-generation concentrated solar power (CSP) plants, with targeted operating temperatures around 750°C. Highly textured single and multimetallic oxide coatings were electrodeposited onto Inconel substrate by systematically varying the composition and process parameters. The optimized coating exhibited micro-to-nano structures designed to match the wavelengths in the visible region of the solar spectrum. These structures facilitate resonant absorption of solar radiation, significantly boosting solar absorption and accommodating thermal stress during high temperature exposure. A high solar absorptance exceeding 0.985 and a low thermal emittance below 0.5, yielding a thermal efficiency near 95%, was achieved for the optimized coatings without any anti-reflective overcoat, that remained robust after 750 h of isothermal exposure to 750°C in air. The coatings are also robust to severe mechanical and environmental stressors. The innovative approach presented in this study demonstrates the potential for tailoring air-stable solar absorber coatings to achieve high absorption, low emittance, and excellent high-temperature endurance, meeting the rigorous demands of next-generation CSP systems. A technoeconomic analysis reveals the economic advantage of the coatings for Gen3 CSP installations in different geographical zones globally.

14 SOLAR ENERGY↗

DOE OSTI2022

The encasulation effect on thermal performance of micro-encapsulated phase change materials during energy absorption

Understanding the performance of the thermal storage materials is required to successfully meet the needs of next generation concentrating solar power projects. This study focuses on the thermal characteristics of the micro-encapsulated phase change material (MEPCM) with metallic core under high temperature. A numerical model was developed and verified to study the transient heat absorption process of MEPCMs made of tin, aluminum and copper core. Convective heat transfer rate, total energy absorption and volumetric energy density were presented. The effect of encapsulation on theses variables was analyzed under various boundary and initial conditions. Its impact on characteristic time variables was discussed. The method presented can be adopted to analyzing both manufacturing and application processes for MEPCMs of various compositions, during which melting and solidification happen. Given certain operating conditions, the results from the model can be referenced to obtain optimal thermal performance of these materials.

Benner, Jingru↗

DOE OSTI2022

Novel fractal-textured solar absorber surfaces for concentrated solar power

The solar absorptance of a thermal receiver surface significantly affects the photothermal conversion efficiency of concentrated solar power (CSP) plants. The development of low-cost Gen3 CSP systems calls for increasing the solar absorptance of the thermal receivers at operating temperatures above 750 °C. This study presents an innovative approach to the fractal, multiscale texturing of absorber surfaces to significantly enhance solar energy absorption for Gen3 CSP applications. The absorber surface is described in terms of its fractal parameters that are uniquely determined from surface profile measurements. The interaction of solar radiation with the fractal surface is numerically simulated by solving the governing Maxwell’s equations for electromagnetic wave propagation to investigate the effect of texturing on the absorptance of the surfaces. It is shown that absorption of the solar spectrum increases with an increase in the fractal dimension and the multiscale asperity height of the surface texturing. Here, the theoretical model is demonstrated to be in close agreement with experimental measurements of spectral absorptance of electrodeposited copper (Cu), copper mono-oxide (CuO), and copper-manganese oxide (CuMnO) surfaces that are textured to produce a range of fractal parameters by tailoring the deposition parameters. Fractal surface texturing is shown to reduce reflectance by over one order of magnitude, yielding an absorptance of greater than 0.985 for CuMnO. For the first time, the study presents a significant effective means of increasing solar absorptance and a fundamental theoretical description of the underlying physics.

14 SOLAR ENERGY↗

DOE OSTI2021

Fiberboard Properties and Degradation Rates for Storage of 9975 Shipping Packages in KAC (2021 Status Report)

Thermal, mechanical, and physical properties have been measured on fiberboard samples following accelerated aging for up to 16 years. The aging environments include elevated temperature up to 250 ºF (the maximum allowed service temperature for fiberboard in 9975 packages) and elevated humidity. Accelerated aging results have been analyzed and used to build aging models. Correlations relating several properties (thermal conductivity, energy absorption, weight, dimensions, and density) to their rate of change in potential storage environments have been developed. Combined with an estimate of the actual conditions the fiberboard experiences in K-Area Complex (KAC), these models allow development of service life predictions. KAC completed calculations that supported extending the service life of 9975 packages with 3013 and non3013 containers in storage from 15 years to 20 years. These calculations addressed the potential for degraded fiberboard properties following 20 years in storage using degradation models developed previously. The updated degradation models developed in this report have been compared to the assumptions in these calculations, and the current results for fiberboard dimensions, density, radial thermal conductivity, and energy absorption remain consistent with those calculations. The axial thermal conductivity degradation rate slightly exceeds calculations estimate of 0.5% per year between 130 and 160 °F. Additional data will continue to be collected to permit future refinements to the models and assumptions. Some of the predicted degradation rates presented in this report are extreme. However, these relate to environments that do not exist within KAC or would be postulated only as upset conditions that would not likely persist for an extended period. For a typical package stored in KAC with approximately 10-12 watts internal heat load or less, and ambient temperatures below 90 ºF, the fiberboard assemblies experience storage conditions less severe than any of the aging environments. Fiberboard in conforming packages with lower internal heat loads should experience little or no degradation and is expected to provide a service life beyond the currently approved 20 year storage period. Packages with higher internal heat loads may not continue to perform their required safety functions beyond 20 years. Ultimately, service life will be determined by the cumulative effect of degradation from all the conditions these packages might encounter. The results and model predictions presented in this report are applicable to 9975 packages with cane or softwood fiberboard overpack assemblies. These degradation models do not address the effects of nonconforming conditions such as the presence of excess moisture and mold or beetle infestations.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2022

Fiberboard Properties and Degradation Rates for Storage of 9975 Shipping Package in KAC (2022 Status Report)

Thermal, mechanical, and physical properties have been measured on fiberboard samples following accelerated aging for up to 17 years. The aging environments include elevated temperature up to 250 °F (the maximum allowed service temperature for fiberboard in 9975 packages) and elevated humidity. Accelerated aging results have been analyzed and used to build aging models. Correlations relating several properties (thermal conductivity, energy absorption, weight, dimensions, and density) to their rate of change in potential storage environments have been developed. Combined with an estimate of the actual conditions the fiberboard experiences in K-Area Complex (KAC), these models allow development of service life predictions. KAC completed calculations that supported extending the service life of 9975 packages with 3013 containers in storage from 20 years to 40 years. These calculations addressed the potential for degraded fiberboard properties following 40 years in storage using degradation models developed previously. Due to differences in containers, 9975 packages with non-3013 containers are only approved for 20 years of storage. The updated degradation models developed in this report have been compared to the assumptions in those calculations, and the current results for fiberboard dimensions, density, radial thermal conductivity, and energy absorption remain consistent with those calculations. The axial thermal conductivity degradation rate slightly exceeds calculations estimate of 0.5% per year between 130 and 160 °F. Additional data will continue to be collected to permit future refinements to the models and assumptions. Some of the predicted degradation rates presented in this report are extreme. However, these relate to environments that do not exist within KAC or would be postulated only as upset conditions that would not likely persist for an extended period. For a typical package stored in KAC with approximately 10-12 watts internal heat load or less, and ambient temperatures below 90 °F, the fiberboard assemblies experience storage conditions less severe than any of the aging environments. Fiberboard in conforming packages with lower internal heat loads should experience little or no degradation and is expected to provide a service life beyond the currently approved 40 year storage period. Packages with higher internal heat loads may not continue to perform their required safety functions beyond 40 years. Ultimately, service life will be determined by the cumulative effect of degradation from all the conditions these packages might encounter. The results and model predictions presented in this report are applicable to 9975 packages with cane or softwood fiberboard overpack assemblies. These degradation models do not address the effects of non-conforming conditions such as the presence of excess moisture and mold or beetle infestations.

36 MATERIALS SCIENCE↗

DOE OSTI2025

2025 Status Report - Fiberboard Properties and Degradation Rates for Storage of 9975 Shipping Package in KAC

Fiberboard assemblies in the 9975 package were identified as susceptible to aging and degradation under long-term storage conditions. Thermal, mechanical, and physical properties have been measured on fiberboard samples aging for up to 20 years at accelerated conditions. The aging environments include elevated temperature up to 250 ºF (the maximum allowed service temperature for fiberboard in 9975 packages) and elevated humidity. Accelerated aging results have been analyzed and used to build aging models. Correlations relating several properties (thermal conductivity, energy absorption, weight, dimensions, and density) to their rate of change in potential storage environments have been developed. Combined with an estimate of the actual conditions the fiberboard experiences in K-Area Complex (KAC), these models allow development of service life predictions. KAC completed calculations that supported extending the service life of 9975 packages with 3013 containers in storage from 20 years to 40 years. These calculations addressed the potential for degraded fiberboard properties following 40 years in storage using degradation models. The 40 year storage evaluations assumed the degradation rates from initial values for density, dimensional, and thermal properties were 0.5% per year (i.e., after 40 years, the density, dimensional, and thermal properties of fiberboard were 80% of its initial values). The updated degradation models developed in this report were compared to the assumptions in those calculations, and the current results for fiberboard dimensions, density, axial and radial thermal conductivities, and energy absorption remain consistent with those calculations. Additional data will continue to be collected to permit future refinements to the models and assumptions. Some of the predicted degradation rates presented in this report are purposely high to accelerate aging. These rates relate to environments that do not exist within KAC or are postulated to only occur as upset conditions that are unlikely to persist for an extended period. For a typical package stored in KAC with approximately 10-12 watts internal heat load or less, and ambient temperatures below 90 ºF, the fiberboard assemblies experience storage conditions less severe than any of the aging environments (i.e., under 125 °F) used in this study. Fiberboard in conforming packages with lower internal heat loads should experience little or no degradation and is expected to provide a service life beyond the currently approved 40 year storage period. Packages with higher internal heat loads may not continue to perform their required safety functions beyond 40 years. Ultimately, service life will be determined by the cumulative effect of degradation from all the conditions these packages might encounter. The results and model predictions presented in this report are applicable to 9975 packages with cane or softwood fiberboard overpack assemblies. These degradation models do not address the effects of nonconforming conditions such as the presence of excess moisture and mold or beetle infestations.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2021

Robust and Spectrally Selective Aerogels for Solar Receivers

The development of next generation concentrated solar thermal (CST) plants requires solar receivers to reach high temperatures (> 600°C) while minimizing costs. Efficiently generating such high temperatures using a line-focusing collector and an air-stable receiver has the potential to change the current CSP paradigm because it would: (1) result in large improvements in system-level efficiency of line-focusing systems by enabling the use of high-efficiency supercritical CO 2 power cycles; (2) decrease the LCOE of line-focusing systems to meet SETO 2030 goals; (3) maintain performance over the lifetime of the CSP plant by avoiding issues related to breakdown of vacuum. The use of aerogels as transparent insulating materials (TIMs) in solar thermal receivers has the potential to enable such improvements. Specifically, aerogels can be placed in front of a black (or partially selective) high-temperature absorber to allow sunlight to transmit to the absorber but block heat from escaping. These materials can improve the efficiency and simplify the complexity of thermal transport systems by enabling operation at moderate or no vacuum levels. These potential benefits have been explicitly identified by SETO as ‘high impact’. The use of mesoporous silica as a TIM has already led to large improvements in solar collection efficiency. Nevertheless, these materials inherently lose structural integrity and the ability to suppress radiation losses at high temperatures. Here, we address these challenges by leveraging 1-cycle atomic layer deposition of aluminum oxide onto a silica aerogel to form a thermally stable interfacial layer that is transparent to sunlight but broadly absorbs in the mid-infrared. This interfacial absorption results in a two-fold reduction in measured heat losses from an absorber at 700°C and solar thermal efficiency of 81% at 700°C under 60 Suns, based on measurements of heat loss and solar transmittance. Extended-duration heat treatment reveals that the multicomponent aerogel is stable at high temperatures relative to a silica aerogel. Furthermore, we experimentally demonstrate the concept of using infrared plasmon resonances to selectively enhance the thermal absorption coefficient of TIMs in order to strongly suppress thermal radiative losses at high temperatures. We term this mechanism plasmon-enhanced greenhouse selectivity (PEGS). Unlike silica aerogels, where much of the IR absorption is lost at high temperatures, local surface plasmon resonances (LSPRs) in doped oxide nanoparticles overlap a significant portion of the blackbody spectrum and are maintained at high temperatures. Overall, this work paves the way for next-generation solar thermal energy using thermally robust transparent insulating materials.

14 SOLAR ENERGY↗

DOE OSTI2020

Robust and Spectrally Selective Aerogels for Solar Receivers (Final Technical Report)

The development of next generation concentrated solar thermal (CST) plants requires solar receivers to reach high temperatures (> 600°C) while minimizing costs. Efficiently generating such high temperatures using a line-focusing collector and an air-stable receiver has the potential to change the current CSP paradigm because it would: (1) result in large improvements in system-level efficiency of line-focusing systems by enabling the use of high-efficiency supercritical CO2 power cycles; (2) decrease the LCOE of line-focusing systems to meet SETO 2030 goals; (3) maintain performance over the lifetime of the CSP plant by avoiding issues related to breakdown of vacuum. The use of aerogels as transparent insulating materials (TIMs) in solar thermal receivers has the potential to enable such improvements. Specifically, aerogels can be placed in front of a black (or partially selective) high-temperature absorber to allow sunlight to transmit to the absorber but block heat from escaping. These materials can improve the efficiency and simplify the complexity of thermal transport systems by enabling operation at moderate or no vacuum levels. These potential benefits have been explicitly identified by SETO as ‘high impact’. The use of mesoporous silica as a TIM has already led to large improvements in solar collection efficiency. Nevertheless, these materials inherently lose structural integrity and the ability to suppress radiation losses at high temperatures. Here, we address these challenges by leveraging 1-cycle atomic layer deposition of aluminum oxide onto a silica aerogel to form a thermally stable interfacial layer that is transparent to sunlight but broadly absorbs in the mid-infrared. This interfacial absorption results in a two-fold reduction in measured heat losses from an absorber at 700°C and solar thermal efficiency of 81% at 700°C under 60 Suns, based on measurements of heat loss and solar transmittance. Extended-duration heat treatment reveals that the multicomponent aerogel is stable at high temperatures relative to a silica aerogel. Furthermore, we experimentally demonstrate the concept of using infrared plasmon resonances to selectively enhance the thermal absorption coefficient of TIMs in order to strongly suppress thermal radiative losses at high temperatures. We term this mechanism plasmon-enhanced greenhouse selectivity (PEGS). Unlike silica aerogels, where much of the IR absorption is lost at high temperatures, local surface plasmon resonances (LSPRs) in doped oxide nanoparticles overlap a significant portion of the blackbody spectrum and are maintained at high temperatures. Overall, this work paves the way for next-generation solar thermal energy using thermally robust transparent insulating materials.

14 SOLAR ENERGY↗

DOE OSTI2023

High-Temperature Air Stability of Electrodeposited Copper Cobalt Oxide and Copper Manganese Oxide Absorber Coatings for Concentrating Solar Power

The solar absorptance of a thermal receiver surface significantly affects the photothermal conversion efficiency of concentrating solar power (CSP) plants. The stability of solar receivers and coatings applied to improve solar absorptance at high temperatures is critical for efficient and long-term operation. This study analyzes the high-temperature air stability of multiscale fractal textured electrodeposited copper manganese oxide and copper cobalt oxide solar receiver coatings over a range of temperatures. The study also investigates the effect of high temperature on phase stability, chemical and morphological evolution, and the optical properties of the two solar absorber materials. A computational model is developed to determine the absorptance of the textured absorbers and is shown to match the experimental measurements closely over a range of heat treatment temperatures from 450 °C to 850 °C and durations up to 100 h. Degradation curves and coating stability maps are developed from the study. Copper manganese oxide and copper cobalt oxide coatings exhibit good thermal stability up to ~815 °C and 630 °C, respectively, with minimal changes in their optical and structural properties with thermal efficiency greater than 90%. Furthermore, the study offers valuable insights into the high-temperature annealing effects on the optical and structural properties of multiscale copper alloyed coatings fabricated by electrodeposition and presents a means of designing the optimal temperature range for maximizing absorber efficiency in practical applications.

14 SOLAR ENERGY↗

DOE OSTI2021

Development and characteristics of ultra high-performance lightweight cementitious composites (UHP-LCCs)

Highlights: • An ultra high-performance lightweight cementitious composite (UHP-LCC) was designed. • The UHP-LCCs had ultra high strength (>120 MPa) and very low density (3 ). • The UHP-LCCs had high structural efficiency, good functional properties and superior durability. • The strategies and mechanisms on achieving UHP-LCCs with excellent performance were proposed. High strength and light weight are two recent opposite development trends of concrete. This study proposed a design concept of an ultra high-performance lightweight cementitious composite (UHP-LCC), which had a compressive strength of higher than 120 MPa and an air-dried density down to around 1800 kg/m{sup 3}. The UHP-LCCs were innovatively developed by incorporating micro-sized hollow particles with a high strength shell (hollow glass microspheres, HGM) into an ultra-high performance cementitious composite (UHPC). The roles of HGM in the UHP-LCCs were investigated by evaluating the reactivity of the HGM and the mechanisms on achieving the excellent mechanical properties, low density and superior durability were revealed. The Chapelle test results showed that the HGM exhibited some pozzolanic reactivity, which facilitated the reaction between the shell of HGM and the alkali hydration products of the paste matrix. This chemical reaction was conducive to improving the HGM-paste interface and enhancing the mechanical properties. With the use of microspheres with a high stiff shell, the fundamental properties of the UHP-LCCs including thermal insulation, sound absorption, resistance to water ingress and electrical resistivity were improved significantly. The strategies for preparing the UHP-LCCs with high structural efficiency and great performance were proposed. The results of this study provide a new approach for designing and producing a lightweight UHPC, which would be a promising material for long-span structures.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Investigation of fouling mechanisms for diesel engine exhaust heat recovery

The effect of diesel engine exhaust fouling on heat and mass exchangers for waste heat recovery is investigated. Experiments are conducted for a range of operating conditions relevant to the use of the waste heat from a diesel engine for powering a 2.71 kW capacity absorption heat pump. Thermal resistances of fouling layers as well as their effects on pressure drop are determined, and the underlying mechanisms for deposition and removal are investigated. Fouling layer effects are most severe for the lowest coolant temperatures and 100% generator load. At these conditions, the fouling thermal resistance is approximately 70% of the total resistance, and the ratio of the steady-state pressure drop to the baseline pressure drop is 3.25. Flow induced shear is found to be the primary growth inhibiting mechanism at high exhaust velocities. Findings from this study can guide heat exchanger design for a variety of waste heat recovery systems.

04 OIL SHALES AND TAR SANDS↗

DOE OSTI2021

Burning velocities of R-32/O 2 /N 2 mixtures: Experimental measurements and development of a validated detailed chemical kinetic model

This work entails characterizing the flammability of the refrigerant R-32 (CH 2 F 2 ) by both experimental measurements and modeling. Burning velocities S u were measured using a constant-volume spherical-flame method for R-32/O2/N 2 mixtures with O 2 /N 2 ratios ranging from 21% (synthetic air) to 40%, pressures of (1 to 3) bar, and equivalence ratios $\phi$ of (0.8 to 1.3). Based on a critical assessment of available data, and extended by our own calculations, a detailed chemical kinetic model was developed and key reactions determined using reaction path and sensitivity analyses. Initiation and combustion were identified as distinct kinetic regimes and burning velocities were found to be controlled by two primary reactions: unimolecular decomposition of CH 2 F 2 → CHF + HF and the subsequent reaction, CHF + O 2 → CHFO + O, the latter reaction initiating the radical chain propagating and branching by producing O atoms. Sensitive rate constants in the kinetic model were critically adjusted within their uncertainties and current knowledge bounds to best fit the experimental burning velocities. We found that rate constants in the model could be adjusted to match a given experimental S u for specific conditions (O 2 loading, P, T, $\phi$). This, however, then fixes predicted burning velocities for other all conditions within (3 to 4)% if physically realistic rate parameters are maintained. Thus, the entire set of experimental data is fit, not just to particular conditions. Relative random uncertainties in the experimental Su measurements were (4 to 6)%, but assumptions made for thermal radiation lost by the burned gas in the spherical-flame experiments add an additional systematic uncertainty. Systematic differences between the limiting cases of adiabatic (no thermal radiation lost) and optically-thin (all thermal radiation lost) varied significantly with conditions and ranged from (4 to 30)% at high to low velocities, respectively, translating into uncertainties of (2 to 15)% considering the average of two limiting cases. Comparison of experimental and kinetically modeled Su values suggests that the burned gas tends towards the optically-thin limit at the lowest pressures and fuel loadings and toward the adiabatic limit at the highest pressures and loadings. We tested and found support for this conclusion with a detailed analysis as a function of all the conditions (T, P, % O 2 , $\phi$). This behavior appears to transition from optically-thin to adiabatic as the density of the initial fuel increases, which results in increased CO 2 in the burned gas and thus increased absorption of the thermal radiation (consistent with the Beer-Lambert Law). The validated detailed model based on evaluated kinetics is shown to accurately predict burning velocities for R-32 O 2 /N 2 mixtures over a wide range of conditions and provides a reliable basis for extrapolation to other conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗