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At least 253 records · Page 14

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DOE OSTI2024

Role of Metal–Organic Framework Topology on Thermodynamics of Polyoxometalate Encapsulation

Polyoxometalates (POMs) are discrete anionic clusters whose rich redox properties, strong Brønsted acidity, and high availability of active sites poise them as potent catalysts for oxidation reactions. Here, metal–organic frameworks (MOFs) have emerged as tunable, porous platforms to immobilize POMs, thus increasing their solution stability and catalytic activity. While POM@MOF composite materials have been widely used for a variety of applications, little is known about the thermodynamics of the encapsulation process. Here, we utilize an up-and-coming technique in the field of heterogeneous materials, isothermal titration calorimetry (ITC), to obtain full thermodynamic profiles (ΔH, ΔS, ΔG, K a ) of POM binding. Six different 8-connected hexanuclear Zr-MOFs were investigated to determine the impact of MOF topology (csq, scu, the) on POM encapsulation thermodynamics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Carbon Nanosphere-Encapsulated Fe Core–Shell Structures for Catalytic CO 2 Hydrogenation

In this work, we synthesized a unique carbon nanosphere (CNS)-encapsulated Fe core–shell catalyst (CNS–Fe) for CO 2 hydrogenation. The synthesized CNS–Fe catalyst exhibited a core–shell structure with a core of ca. 40 nm containing iron species and a shell thickness of ca. 10 nm composed of mainly graphitic carbon. X-ray diffraction, X-ray photoelectron spectroscopy, Raman spectroscopy, and thermogravimetric analysis were used to characterize the fresh and spent CNS–Fe catalysts and reveal a mixture of Fe 3 O 4 , metallic Fe, and Fe 5 C 2 in the core and graphitic carbon as the shell with defect sites. Hydrogen temperature-programmed reduction, X-ray absorption near-edge structure, and extended X-ray absorption fine structure for the fresh CNS–Fe confirmed the composition of the iron species encapsulated in the CNS. The catalytic performance of CNS–Fe was investigated at ambient pressure for CO2 hydrogenation with hydrocarbons (CH 4 , C 2 –C 4 = , C 2 –C 4 0 ), and CO was observed as the main product.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Probing the active sites of oxide encapsulated electrocatalysts with controllable oxygen evolution selectivity

Electrocatalysts encapsulated by nanoscopic overlayers can control the rate of redox reactions at the outer surface of the overlayer or at the buried interface between the overlayer and the active catalyst, leading to complex behavior in the presence of two competing electrochemical reactions. This study investigated oxide encapsulated electrocatalysts (OECs) comprised of iridium (Ir) thin films coated with an ultrathin (2–10 nm thick) silicon oxide (SiO x ) or titanium oxide (TiO x ) overlayer. The performance of SiO x |Ir and TiO x |Ir thin film electrodes towards the oxygen evolution reaction (OER) and Fe(II)/Fe(III) redox reactions were evaluated. An improvement in selectivity towards the OER was observed for all OECs. Overlayer properties, namely ionic and electronic conductivity, were assessed using a combination of electroanalytical methods and molecular dynamics simulations. SiO x and TiO x overlayers were found to be permeable to H 2 O and O 2 such that the OER can occur at the MO x |Ir (M = Ti, Si) buried interface, which was further supported with molecular dynamics simulations of model SiO 2 coatings. In contrast, Fe(II)/Fe(III) redox reactions occur to the same degree with TiO x overlayers having thicknesses less than 4 nm as bare electrocatalyst, while SiO x overlayers inhibit redox reactions at all thicknesses. This observation is attributed to differences in electronic transport between the buried interface and outer overlayer surface, as measured with through-plane conductivity measurements of wetted overlayer materials. These findings reveal the influence of oxide overlayer properties on the activity and selectivity of OECs and suggest opportunities to tune these properties for a wide range of electrochemical reactions.

08 HYDROGEN↗

DOE OSTI2015

Thin-film encapsulation of the air-sensitive organic-based ferrimagnet vanadium tetracyanoethylene

The organic-based ferrimagnet vanadium tetracyanoethylene (V[TCNE]{sub x∼2}) has demonstrated potential for use in both microwave electronics and spintronics due to the combination of high temperature magnetic ordering (T{sub C} > 600 K), extremely sharp ferromagnetic resonance (peak to peak linewidth of 1 G), and low-temperature conformal deposition via chemical vapor deposition (deposition temperature of 50 °C). However, air-sensitivity leads to the complete degradation of the films within 2 h under ambient conditions, with noticeable degradation occurring within 30 min. Here, we demonstrate encapsulation of V[TCNE]{sub x∼2} thin films using a UV-cured epoxy that increases film lifetime to over 710 h (30 days) as measured by the remanent magnetization. The saturation magnetization and Curie temperature decay more slowly than the remanence, and the coercivity is unchanged after 340 h (14 days) of air exposure. Fourier transform infrared spectroscopy indicates that the epoxy does not react with the film, and magnetometry measurements show that the presence of the epoxy does not degrade the magnetic properties. This encapsulation strategy directly enables a host of experimental protocols and investigations not previously feasible for air-sensitive samples and lays the foundation for the development of practical applications for this promising organic-based magnetic material.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2015

Ab-initio study of encapsulated and functionalized silicon nanotube with a monoatomically thin Cu wire

First principle calculations based on DFT have been performed to study the interaction of monoatomically thin Cu wire with silicon nanotube in armchair configuration having chirality (6, 6) both by placing it inside (encapsulation) and outside (functionalisation) the tube. The lowest energy for positioning monoatomically thin Cu wire inside and outside surfaces of SiNT were found to possess cohesive energies of 4.03 eV and 4.02 eV respectively and hence the stability of both SiNTs is found to be almost same. However, From the electronic band structures study, the conductance in case of SiNT for the encapsulated and functionalized positioning of the Cu wire have been found to be 2G{sub 0} and 4G{sub 0} respectively showing enhanced conductance for the functionalized SiNT.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2015

Morphology of a columnar stack of coronene molecules encapsulated in a single-walled carbon nanotube

The morphology of stacked coronene molecules encapsulated in a single-walled carbon nanotube (SWCNT) is investigated using atomistic simulation. First, the minimum energy configuration of coronene molecules in a SWCNT is sought by means of conjugate gradient (CG) minimization. Secondly, encapsulation of coronene molecules into a SWCNT existing in a coronene atmosphere is simulated by means of molecular dynamics (MD). In both of the simulations, the diameter of the SWCNT ranges from 1.35 to 1.69 nm, and the final configurations of coronene molecules within a SWCNT are examined. In a thin SWCNT, coronene molecules tilt against the radial direction of the SWCNT and slide relative to each other, whereas in a thick SWCNT, they do not tilt but rotate relative to each other. In a SWCNT of the intermediate diameter, they tilt, slide, and rotate. For the SWCNT diameter less than or equal to 1.52 nm, the mean tilt angle of the stacked coronene molecules almost linearly decreases with increasing the diameter, whereas for the diameter above 1.52 nm, it is approximately 0{sup ∘}. To check the validity of the results, the MD simulations are performed changing the density of the coronene atmosphere and the length of the SWCNT; the results prove to be valid. Finally, the effects of temperature on the mean tilt angle and mean intermolecular distance of stacked coronene molecules are examined by a rather simplified simulation, which shows that both of them increase with increasing temperature.

36 MATERIALS SCIENCE↗

DOE OSTI2017

Encapsulant Adhesion to Surface Metallization on Photovoltaic Cells

Delamination of encapsulant materials from PV cell surfaces often appears to originate at regions with metallization. Using a fracture mechanics based metrology, the adhesion of ethylene vinyl acetate (EVA) encapsulant to screen-printed silver metallization was evaluated. At room temperature, the fracture energy Gc [J/m2] of the EVA/silver interface (952 J/m2) was ~70% lower than that of the EVA/antireflective (AR) coating (>2900 J/m2) and ~60% lower than that of the EVA to the surface of cell (2265 J/m2). After only 300 h of damp heat aging, the adhesion energy of the silver interface dropped to and plateaued at ~50-60 J/m2 while that of the EVA/AR coating and EVA/cell remained mostly unchanged. Elemental surface analysis showed that the EVA separates from the silver in a purely adhesive manner, indicating that bonds at the interface were likely displaced in the presence of humidity and chemical byproducts at elevated temperature, which in part accounts for the propensity of metalized surfaces to delaminate in the field.

14 SOLAR ENERGY↗

DOE OSTI2021

Nanomechanical and Fluorescence Characterizations of Weathered PV Module Encapsulation

Nanoindentation and fluorescence spectroscopy provide spatially resolved mechanical and chemical characterization for degradation of poly (ethylene-co-vinyl acetate) (EVA) encapsulants aged under accelerated weathering and in field deployed photovoltaic (PV) modules. For the accelerated weathering tests, two different EVA formulations in the glass/EVA/glass-laminated coupons were exposed to ultraviolet (UV) light for 180 days at three different temperatures (40, 60, and 80 °C) and UV intensities (0.4, 2.2, and 2.9 W/m2/nm at 340 nm). The fluorescence spectra and moduli were uniform through the cross section of both EVA formulations at the lowest temperature and UV intensity; however, under the highest temperature and UV intensity, the UV irradiated sides showed lower moduli and higher fluorescence compared to the opposite sides. For EVA obtained from PV modules deployed 27 years in Sacramento, CA, USA, changes in fluorescence intensity across the thickness were relatively greater than changes in modulus. On the other hand, for EVA obtained from the same type of module stored in the shed for 27 years, no fluorescence was observed, and a uniform modulus was seen through the EVA layer, but with substantially higher values than those obtained from the field-deployed modules. The different extent of changes between laboratory and field exposures suggests the importance of considering effects of temperature and UV intensity for designing a reliable accelerated testing. This study uniquely demonstrates the capability of microscale characterization using nanoindentation and fluorescence microscopy to monitor mechanical and chemical degradation of EVA encapsulants in PV modules.

14 SOLAR ENERGY↗

DOE OSTI2018

Activation Energy Determination for Photovoltaic Encapsulant Discoloration by Indoor Accelerated UV Testing

A novel methodology for determining the activation energy of photovoltaic encapsulant discoloration using an indoor accelerated ultraviolet (UV) stress test while simultaneously maintaining multiple module temperatures in a single weathering chamber is presented. The testing was performed on some fresh mini-modules with a glass/EVA/cell/EVA/backsheet construction. The short-circuit current degradation from individual cells was used to quantify transmittance losses due to discoloration. Activation energy determined using indoor accelerated UV test data and Modified Arrhenius model ranges from 26 to 44 kJ/mol (0.27 to 0.46 eV). Activation energy was also determined from the outdoor field degradation data by employing different physical models that consider the individual or combined effects of key environmental factors. The approach here is instrumental to evaluating the reliability studies on encapsulant degradation mechanisms using relatively less time and resources.

14 SOLAR ENERGY↗

DOE OSTI2014

Nondestructive Assay Options for Spent Fuel Encapsulation

This report describes the role that nondestructive assay (NDA) techniques and systems of NDA techniques may have in the context of an encapsulation and deep geological repository. The potential NDA needs of an encapsulation and repository facility include safeguards, heat content, and criticality. Some discussion of the facility needs is given, with the majority of the report concentrating on the capability and characteristics of individual NDA instruments and techniques currently available or under development. Particular emphasis is given to how the NDA techniques can be used to determine the heat production of an assembly, as well as meet the dual safeguards needs of 1) determining the declared parameters of initial enrichment, burn-up, and cooling time and 2) detecting defects (total, partial, and bias). The report concludes with the recommendation of three integrated systems that might meet the combined NDA needs of the encapsulation/repository facility.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2013

Measure Guideline: Buried and/or Encapsulated Ducts

Buried and/or encapsulated ducts (BEDs) are a class of advanced, energy-efficiency strategies intended to address the significant ductwork thermal losses associated with ducts installed in unconditioned attics. BEDs are ducts installed in unconditioned attics that are covered in loose-fill insulation and/or encapsulated in closed cell polyurethane spray foam insulation. This Measure Guideline covers the technical aspects of BEDs as well as the advantages, disadvantages, and risks of BEDs compared to other alternative strategies. This guideline also provides detailed guidance on installation of BEDs strategies in new and existing homes through step-by-step installation procedures. This Building America Measure Guideline synthesizes previously published research on BEDs and provides practical information to builders, contractors, homeowners, policy analysts, building professions, and building scientists. Some of the procedures presented here, however, require specialized equipment or expertise. In addition, some alterations to duct systems may require a specialized license. Persons implementing duct system improvements should not go beyond their expertise or qualifications. This guideline provides valuable information for a building industry that has struggled to address ductwork thermal losses in new and existing homes. As building codes strengthen requirements for duct air sealing and insulation, flexibility is needed to address energy efficiency goals. While ductwork in conditioned spaces has been promoted as the panacea for addressing ductwork thermal losses, BEDs installations approach - and sometimes exceed - the performance of ductwork in conditioned spaces.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

DOE OSTI2013

Measure Guideline: Buried and/or Encapsulated Ducts

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

DOE OSTI2021

Ultra-High-Performance Grout for Encapsulation of HEPA Filters

Ultra-high-performance grout (UHPG) grout appears to be good candidate for solidification and encapsulation of waste containing 99 Tc and 129 I that benefits from low Dobs. The properties that make UHPG a good candidate for encapsulating HEPA filters would make it a good option for microencapsulating other solid secondary waste (SSW) such as granular activated carbon, silver mordenite, and ion exchange resins. Containers made of UHPG would also be good candidates for dry disposal of SSW due to its very low diffusivity which prevents contaminant migration.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2025

Gel Permeation Chromatography on commercial source encapsulants under thermal accelerated aging

Gel permeation chromatography analysis of the uncrosslinked portions of polymeric encapsulants (EVA, POE, EPE) aged under thermal accelerated aging conditions (in the absence of UV) is not a reliable way to measure encapsulant crosslinking nor degradation

accelerated aging↗

NASA NTRSDate not supplied

Single-Cell Analysis of Yeast (Saccharomyces cerevisiae) Using Hydrogel Encapsulation

Space radiation poses a major health risk to astronauts. To fulfill NASA’s mission of exploration beyond Earth, the biological effects of Galactic Cosmic Radiation and gamma radiation must be investigated to elucidate cellular damage mechanisms and inform countermeasure protocols to safely bring humans beyond Earth’s magnetosphere. Budding yeast (Saccharomyces cerevisiae) are commonly used in experiments as a model organism for studying the effects of radiation on eukaryotes. Radiobiology of yeast at the single cell level is poorly understood, yet crucial for informing models to aid in the design and interpretation of experiments. We are using a novel method of microencapsulation in hydrogel particles (PicoShells) to enable analysis of the distribution of radiation-induced damage among yeast cells at the single-cell level, in high throughput. Here we describe the development of methods for culturing, visualization, and quantification of encapsulated yeast. The encapsulated yeast are cultured in Yeast extract-Peptone-Dextrose (YPD) medium, fixed in formaldehyde or ethanol, and stained with DAPI or propidium iodide, then visualized using microscopy or enumerated using flow cytometry, with the aim of developing a protocol to enumerate the distribution of viable cells in each PicoShell. This will allow us to quantify how different forms of radiation can generate different distributions of damage across a population of cells, ultimately providing insight into the biological effects of space-relevant ionizing radiation.

yeast↗

DOE OSTI2013

Technology Solutions Case Study: Buried and Encapsulated Ducts, Jacksonville, Florida

Ductwork installed in unconditioned attics can significantly increase the overall heating and cooling costs of residential buildings. In fact, estimated duct thermal losses for single-family residential buildings with ductwork installed in unconditioned attics range from 10% to 45%. In a study of three single-story houses in Florida, the Building America research team Consortium for Advanced Residential Buildings (CARB) investigated the strategy of using buried and/or encapsulated ducts (BED) to reduce duct thermal losses in existing homes. The BED strategy consists of burying ducts in loose-fill insulation and/or encapsulating them in closed cell polyurethane spray foam (ccSPF) insulation; specifically for use in humid climates.

attics↗

DOE OSTI2017

Evaluation of Encapsulant Adhesion to Surface Metallization of Photovoltaic Cells: Preprint

Delamination of encapsulant materials from PV cell surfaces often appears to originate at regions with metallization. Using a fracture mechanics based metrology, the adhesion of EVA encapsulant to screen printed silver metallization was evaluated. At room temperature, the fracture energy, Gc [J/m2], of the EVA/silver interface (952 J/m2) was ~70% lower than that of the EVA/AR coating (>2900 J/m2) and ~60% lower than that of the EVA to the surface of cell (2265 J/m2). After only 300 hours of damp heat aging, the adhesion energy of the silver interface dropped to and plateaued at ~50-60 J/m2, while that of the EVA/AR coating and EVA/cell remained mostly unchanged. Elemental surface analysis showed that the EVA separates from the silver in a purely adhesive manner, indicating that bonds at the interface were likely displaced in the presence of humidity and elevated temperature, and may explain the propensity for delamination to occur at metallized surfaces in the field.

14 SOLAR ENERGY↗

DOE OSTI2015

Encapsulation of ILW metals by melting technology - 15360

This paper outlines how encapsulation using melting technology can be performed and describe the positive effects in a handling and repository perspective. Based on a feasibility study of a conditioning method for reactor core components and other ILW metals with a high content of long-lived radionuclides, the paper gives an overview of the concept and how the method can be facilitated. The paper covers identification and analysis of alternative techniques that supports the aim from a repository perspective, which is to strengthen the defense in depth for long-lived waste to be disposed. Embedding of radioactive metallic ILW components can isolate the activated component from corrosion and leakage of radionuclides into the repository barrier systems. By implementing a system that delays the mobility of nuclides the leakage to the biosphere can be delayed and by then decreased significantly. Conditioning by embedding has potential to strengthen a repository concept significantly. It may in certain cases also reduce the requirements on the repository barriers. In addition to the above, embedding also serves as an efficient radiation protection, which simplifies post treatment handling of the waste. The concept can be applied on a wide spectrum of metallic components. Positive effects in a handling and repository perspective can be achieved if low level metal not subject to free release is used as embedding material, since conditioning of metallic ILW waste can be carried out at significant lower dose rates and without increasing the total amount to be disposed. The paper discuss why there are embedding alternatives for ILW metals that are considered to be both technically feasible and reasonable in cost both with regards to investment and operational cost. A cost-benefit analysis as well as a risk analysis is discussed in order to support the feasibility assessment of a facility for encapsulation of ILW metals by melting technology. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗