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At least 937 records · Page 52

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DOE OSTI2013

Containment at the Source during Waste Volume Reduction of Large Radioactive Components Using Oxylance High-Temperature Cutting Equipment - 13595

As a waste-volume reduction and management technique, highly contaminated Control Element Drive Mechanism (CEDM) housings were severed from the Reactor Pressure Vessel Head (RPVH) inside the San Onofre Unit 2 primary containment utilizing Oxylance high-temperature cutting equipment and techniques. Presented are relevant data concerning: - Radiological profiles of the RPVH and individual CEDMs; - Design overviews of the engineering controls and the specialized confinement housings; - Utilization of specialized shielding; - Observations of apparent metallurgical-contamination coalescence phenomena at high temperatures resulting in positive control over loose-surface contamination conditions; - General results of radiological and industrial hygiene air sampling and monitoring; - Collective dose and personnel contamination event statistics; - Lessons learned. (author)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2016

Niagara Falls Storage Site - Interim Waste Containment Structure - 16199

The Niagara Falls Storage Site (NFSS) is a 77.3-hectare (ha) (191-acre) property that is owned by the United States Government and located in the township of Lewiston, Niagara County, New York. The NFSS is part of the former Lake Ontario Ordnance Works (LOOW) that was used by the War Department beginning in 1942 for the production of trinitrotoluene (TNT). During the 1940's and 1950's, the Manhattan Engineer District and the Atomic Energy Commission brought various radioactive wastes and uranium processing byproducts (residues) resulting from our nation's atomic energy program to the LOOW for storage. Site operations caused soil, sediment, and groundwater contamination that lead to several remedial actions, which culminated in the construction of the Interim Waste Containment Structure (IWCS) on the NFSS. The U.S. Army Corps of Engineers (USACE)-Buffalo District is the lead Federal agency for Formerly Utilized Sites Remedial Action Program (FUSRAP) remediation of the NFSS. As the lead agency, USACE is conducting a remedial investigation/feasibility study (RI/FS) pursuant to the protocols set forth in the Comprehensive Environmental Response, Compensation, and Liability Act (CERCLA). CERCLA activities at the NFSS have transitioned from the site RI activities to the FS evaluation of potential remediation alternatives. USACE recognizes the need to implement a focused CERCLA FS process and, therefore, has established three separate operable units (OUs) for NFSS: the IWCS OU, the Balance of Plant (BOP) OU [i.e., all on-site areas outside the boundary of the IWCS], and the Groundwater OU. This paper will discuss the following: - Provide background information on the NFSS including the nature of the materials within the IWCS. - Explain the steps of the CERCLA and associated processes the Formerly Utilized Sites Remedial Action Program (FUSRAP) employs. - Describe the OUs for the NFSS property and the subunit designations used in the FS evaluations for the IWCS OU. - Provide the current project status within the CERCLA framework and path forward for all OUs and Vicinity Properties (VPs). Identify the Applicable or Relevant and Appropriate Requirements (ARARs) preferred by USACE and the regulatory agencies and explain the differences between the two positions. - Provide the comparative evaluation of the remedial alternatives assessed in the FS. - Identify the justifications for the USACE - Buffalo District selecting the preferred remedial alternative within the Proposed Plan. The remedial action objectives for the IWCS OU are designed to provide short- and long-term protection of human health and the environment. CERCLA requires that any action taken be protective of human health and the environment as well as be compliant with identified ARARs. USACE evaluated 'No Action' and four potential remedial alternatives for the IWCS OU that ranged from leaving all of the wastes in-place and installing a final cover to partial and full removal of the contents. The four alternatives met the remedial action objectives defined identified for the IWCS OU. In accordance with the statutory requirements of CERCLA Section 121, remedial alternatives must comply with two threshold criteria, overall protection of human health and the environment and compliance with ARARs, in order to be carried forward for further evaluation. If a remedial alternative meets the threshold criteria, it is evaluated against the following five balancing criteria: - Long-term effectiveness and permanence; - Reduction in toxicity, mobility, or volume through treatment; - Short-term effectiveness; - Implementability; and, - Cost. The Feasibility Study evaluation led to the preferred remedial alternative selection and this will be the focus of this paper. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2016

Experimental Seismic Response of Scaled Storage Containments under Identical Loading Conditions - 16318

Dry Storage Casks (DSCs) store spent nuclear fuel (SNF), usually at sites contiguous to nuclear power plants known as Independent Spent Fuel Storage Installation (ISFSI). DSCs have been considered as a temporary storage solution, and are usually licensed for 20 years, which can be extended up to an operating periods of 60 years. Recently, however, DSCs have been considered as a potential mid-term solution for hundreds of years. This consideration requires reevaluation of DSC performance under a larger seismic hazard. That leads to larger horizontal and vertical accelerations. This study is a part of a research project evaluating the seismic response of free-standing DSCs under long return period seismic events. This article assess whether the response of free-standing structures under seismic excitation is repeatable. For this purpose, experimental tests were conducted using a six degree-of-freedom (6DOF) shake table. During the experimental tests, several ground motions were repeated multiple times to obtain the dynamic response under identical loading conditions. Scaled casks of four aspect ratios (radius to centroidal height ratio, r/h{sub cg}) were studied: 0.39, 0.43, 0.55 and 0.62. The specimens studied are considered to be 1:2.5 and 1:3.5 scaled model of generic prototype casks. The experimental results show that a small change in initial conditions leads to change in the boundary condition of moving bodies and in combination with acceleration being applied at different frequencies contained within the applied ground motions may lead to a large variation in the response. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2019

Engineered Containment Mound (ECM) Design for LLRW at CNL in Chalk River, Canada - 19123

The Atomic Energy of Canada Limited has an initiative to transform the Chalk River Laboratory (CRL) facility into an updated research facility to continue nuclear energy and other energy research which is paramount to the continued growth of the energy sector in Canada. The Near Surface Disposal Facility (NSDF) will be licensed by Canadian Nuclear Safety Commission prior to construction and receipt of waste. The NSDF has been designed to allow for disposal of waste in a manner that is protective of the environment and human health. The Engineered Containment Mound (ECM) is a major structure associated with the NSDF design to allow for long-term disposal of 1,000,000 cubic meters of LLRW. This paper describes the design of major components of the ECM: ECM geometry, perimeter berm, base liner system, and cover system. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2019

Corrosion of Carbon Steel Inside Used Nuclear Fuel Containers - 19492

This paper presents an overview of the carbon steel (CS) corrosion research being conducted by the Radiation Assisted Materials Performance Science (RAMPS) group at Western University, in collaboration with the Canadian Nuclear Waste Management Organization (NWMO) and Canada Natural Science and Engineering Research Council (NSERC). The objective of our studies is to develop a high-fidelity CS corrosion dynamic model that can be used to assess the integrity of the current Canadian used fuel container (UFC) design with confidence. Our key findings, the implications of the findings on corrosion science in general, and the potential consequences of these results on the predictions for long-term UFC integrity are described. Results are presented on the following five themes: chemical kinetics of γ-radiolysis of liquid water and humid air, aqueous corrosion of CS under γ-radiation, corrosion of CS under small water volumes and water filled gaps, Liesegang ring formation in a gel medium, and radiation-induced iron oxide nanoparticle formation from dissolved metal ions. These studies together represent a detailed and integrated examination of the whole CS corrosion system, and in particular, its behaviour under γ-radiation. The key finding of this research is that under certain conditions, the CS corrosion system can exhibit non-linear dynamic behaviours - which can be seen in periodic precipitation patterns and oscillations in measurable system properties such as corrosion potential. This throws into question existing corrosion models that do not account for these types of behaviours. We describe the preliminary steps we have taken in integrating these new understandings into a CS corrosion dynamic model that will be able to make long-term predictions of CS corrosion in the UFC environment. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2017

Formation of Polymeric Nanocubes by Self‐Assembly and Crystallization of Dithiolane‐Containing Triblock Copolymers

Abstract Template‐free fabrication of non‐spherical polymeric nanoparticles is desirable for various applications, but has had limited success owing to thermodynamic favorability of sphere formation. Herein we present a simple way to prepare cubic nanoparticles of block copolymers by self‐assembly from aqueous solutions at room temperature. Nanocubes with edges of 40–200 nm are formed spontaneously on different surfaces upon water evaporation from micellar solutions of triblock copolymers containing a central poly(ethylene oxide) block and terminal trimethylene carbonate/dithiolane blocks. These polymers self‐assemble into 28±5 nm micelles in water. Upon drying, micelle aggregation and a kinetically controlled crystallization of central blocks evidently induce solid cubic particle formation. An approach for preserving the structures of these cubes in water by thiol‐ or photo‐induced crosslinking was developed. The ability to solubilize a model hydrophobic drug, curcumin, was also explored.

Margulis, Katherine↗

DOE OSTI2019

Site-Selective Functionalization of (sp 3 )C-H Bonds Catalyzed by Artificial Metalloenzymes Containing an Iridium-Porphyrin Cofactor

The selective functionalization of one C-H bond over others in nearly identical steric and electronic environments can facilitate the construction of complex molecules. We report site-selective functionalizations of C-H bonds, differentiated solely by remote substituents, catalyzed by artificial metalloenzymes (ArMs) that are generated from the combination of an evolvable P450 scaffold and an iridium-porphyrin cofactor. The generated systems catalyze the insertion of carbenes into the C-H bonds of a range of phthalan derivatives containing substituents that render the two methylene positions in each phthalan inequivalent. These reactions occur with site-selectivity ratios of up to 17.8:1 and, in most cases, with pairs of enzyme mutants that preferentially form each of the two constitutional isomers. This study demonstrates the potential of abiotic reactions catalyzed by metalloenzymes to functionalize C-H bonds with site selectivity that is difficult to achieve with small-molecule catalysts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2019

An Americium‐Containing Metal–Organic Framework: A Platform for Studying Transplutonium Elements

Abstract The synthesis, structure, and spectroscopic characterization of the first transplutonium metal–organic framework (MOF) is described. The preparation and structure of Am‐GWMOF‐6, [Am 2 (C 6 H 8 O 4 ) 3 (H 2 O) 2 ][(C 10 H 8 N 2 )], is analogous to that of the isostructural trivalent lanthanide‐only containing material GWMOF‐6. The presented MOF architecture is used as a platform to probe Am 3+ coordination chemistry and guest‐enhanced luminescent emission, whereas the framework itself provides a means to monitor the effects of self‐irradiation upon crystallinity over time. Presented here is a discussion of these properties and the opportunities that MOFs provide in the structural and spectroscopic study of actinides.

Ridenour, J. August↗

DOE OSTI2021

Heterometallic Actinide‐Containing Photoresponsive Metal‐Organic Frameworks: Dynamic and Static Tuning of Electronic Properties

Abstract Acquiring fundamental knowledge of properties of actinide‐based materials is a necessary step to create new possibilities for addressing the current challenges in the nuclear energy and nuclear waste sectors. In this report, we established a photophysics–electronics correlation for actinide‐containing metal‐organic frameworks (An‐MOFs) as a function of excitation wavelength, for the first time. A stepwise approach for dynamically modulating electronic properties was applied for the first time towards actinide‐based heterometallic MOFs through integration of photochromic linkers. Optical cycling, modeling of density of states near the Fermi edge, conductivity measurements, and photoisomerization kinetics were employed to shed light on the process of tailoring optoelectronic properties of An‐MOFs. Furthermore, the first photochromic MOF‐based field‐effect transistor, in which the field‐effect response could be changed through light exposure, was constructed. As a demonstration, the change in current upon light exposure was sufficient to operate a two‐LED fail‐safe indicator circuit.

Martin, Corey R.↗

DOE OSTI2016

Solvent Extraction: Structure of the Liquid-Liquid Interface Containing a Diamide Ligand

Knowledge of the (supra)molecular structure of an interface that contains amphiphilic ligand molecules is necessary for a full understanding of ion transfer during solvent extraction. Even if molecular dynamics already yield some insight in the molecular configurations in solution, hardly any experimental data giving access to distributions of both extractant molecules and ions at the liquid–liquid interface exist. Here, the combined application of X-ray and neutron reflectivity measurements represents a key milestone in the deduction of the interfacial structure and potential with respect to two different lipophilic ligands. Indeed, we show for the first time that hard trivalent cations can be repelled or attracted by the extractant-enriched interface according to the nature of the ligand.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2016

Nitrosylation of Nitric-Oxide-Sensing Regulatory Proteins Containing [4Fe-4S] Clusters Gives Rise to Multiple Iron-Nitrosyl Complexes

The reaction of protein-bound iron–sulfur (Fe-S) clusters with nitric oxide (NO) plays key roles in NO-mediated toxicity and signaling. Elucidation of the mechanism of the reaction of NO with DNA regulatory proteins that contain Fe-S clusters has been hampered by a lack of information about the nature of the iron-nitrosyl products formed. Herein, we report nuclear resonance vibrational spectroscopy (NRVS) and density functional theory (DFT) calculations that identify NO reaction products in WhiD and NsrR, regulatory proteins that use a [4Fe-4S] cluster to sense NO. This work reveals that nitrosylation yields multiple products structurally related to Roussin's Red Ester (RRE, [Fe 2 (NO) 4 (Cys) 2 ]) and Roussin's Black Salt (RBS, [Fe 4 (NO) 7 S 3 ]. In the latter case, the absence of 32 S/ 34 S shifts in the Fe-S region of the NRVS spectra suggest that a new species, Roussin's Black Ester (RBE), may be formed, in which one or more of the sulfide ligands is replaced by Cys thiolates.

Serrano, Pauline N.↗

DOE OSTI2017

Formation of Polymeric Nanocubes by Self-Assembly and Crystallization of Dithiolane-Containing Triblock Copolymers

Template–free fabrication of non–spherical polymeric nanoparticles is desirable for various applications, but has had limited success owing to thermodynamic favorability of sphere formation. Herein we present a simple way to prepare cubic nanoparticles of block copolymers by self–assembly from aqueous solutions at room temperature. Nanocubes with edges of 40–200 nm are formed spontaneously on different surfaces upon water evaporation from micellar solutions of triblock copolymers containing a central poly(ethylene oxide) block and terminal trimethylene carbonate/dithiolane blocks. These polymers self–assemble into 28±5 nm micelles in water. Upon drying, micelle aggregation and a kinetically controlled crystallization of central blocks evidently induce solid cubic particle formation. An approach for preserving the structures of these cubes in water by thiol– or photo–induced crosslinking was developed. In conclusion, the ability to solubilize a model hydrophobic drug, curcumin, was also explored.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2019

Site-Selective Functionalization of (sp 3 )C-H Bonds Catalyzed by Artificial Metalloenzymes Containing an Iridium-Porphyrin Cofactor

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2019

Analysis of Powders Containing Illicit Drugs Using Magnetic Levitation

Magneto-Archimedes levitation (MagLev) enables the separation of powdered mixtures of illicit drugs (cocaine, methamphetamine, heroin, fentanyl, and its analogues), adulterants, and diluents based on density, and allows the presumptive identification of individual components. Small samples (mass <50 mg), with low concentrations of illicit drugs, present a particular challenge to analysis for forensic chemists. The MagLev device, a cuvette containing a solution of paramagnetic gadolinium(III) chelate in a non-polar solvent, placed between two like-poles-facing NdFeB magnets, allowed separation of seven relevant compounds simultaneously. In particular, initial separation with MagLev, followed by characterization by FTIR-ATR, enabled identification of fentanyl in a sample of fentanyl-laced heroin (1.3 wt % fentanyl, 2.6 wt % heroin, and 96.1 wt % lactose). MagLev allows identification of unknown powders in mixtures and enables confirmatory identification based on structure-specific techniques.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Heterometallic Actinide-Containing Photoresponsive Metal-Organic Frameworks: Dynamic and Static Tuning of Electronic Properties

Acquiring fundamental knowledge of properties of actinide-based materials is a necessary step to create new possibilities for addressing the current challenges in the nuclear energy and nuclear waste sectors. Here in this report, we established a photophysics–electronics correlation for actinide-containing metal-organic frameworks (An-MOFs) as a function of excitation wavelength, for the first time. A stepwise approach for dynamically modulating electronic properties was applied for the first time towards actinide-based heterometallic MOFs through integration of photochromic linkers. Optical cycling, modeling of density of states near the Fermi edge, conductivity measurements, and photoisomerization kinetics were employed to shed light on the process of tailoring optoelectronic properties of An-MOFs. Furthermore, the first photochromic MOF-based field-effect transistor, in which the field-effect response could be changed through light exposure, was constructed. As a demonstration, the change in current upon light exposure was sufficient to operate a two-LED fail-safe indicator circuit.

36 MATERIALS SCIENCE↗

DOE OSTI2019

Matrix Extension Validation of AOCS Ce 2c‐11 for Omega‐3 Polyunsaturated Fatty Acids in Conventional Foods and Dietary Supplements Containing Added Marine Oil

Abstract Marine oils are commonly added to conventional foods and dietary supplements to enhance their contents of omega‐3 polyunsaturated fatty acids (PUFA), including eicosapentaenoic acid (EPA; 20:5n‐3) and docosahexaenoic acid (DHA; 22:6n‐3), which have been associated with numerous potential health benefits. This study compared American Oil Chemists’ Society (AOCS) Official Methods Ce 2b‐11 and Ce 2c‐11 for determining EPA and DHA in foods and dietary supplements and found that AOCS Ce 2c‐11 produces significantly higher analyzed values, which could be attributed to a more comprehensive breakdown of the sample matrix and derivatization of fatty acids. Our subsequent food matrix extension validation of AOCS Ce 2c‐11 demonstrated that the method produces true, accurate, sensitive, and precise determinations of EPA, DHA, and total omega‐3 PUFA in foods and dietary supplements containing added marine oil, including those formulated with emulsified and microencapsulated oils. The method detection limits for EPA and DHA were 0.012 ± 0.002 and 0.011 ± 0.003 mg g −1 , respectively (means ± SD). The analyzed contents of EPA (1.26–386 mg serving −1 ), DHA (1.37–563 mg serving −1 ), and total omega‐3 PUFA (2.69–1270 mg serving −1 ) were reported for 27 conventional food and dietary supplement products. Eighteen products declared contents of DHA, EPA + DHA, or total omega‐3 PUFA on product labels, and the analyzed contents of those fatty acids varied from 95 to 162% of label declarations for all but two of the products.

Li, Ziyi↗

DOE OSTI2022

Interlaminar improvement of carbon fiber/epoxy composites via fluorine‐containing high‐epoxy‐value sizing agent

Abstract To improve the interfacial bonding effect of carbon fibers (CFs) and epoxy resins, we prepared a fluorine‐containing high‐epoxy‐value sizing agent (named TS) in this article. It is an emulsion with a more uniform particle size distribution and higher stability better than a commercial Takemoto sizing agent. In addition, sulfonic acid groups can improve the hydrophilicity of the TS, and the presence of epoxy groups enhances the wettability between CFs and the matrix. The properties of the sizing agents were examined by Fourier transform infrared spectroscopy, dynamic light scattering, and thermogravimetric analysis. The sized CFs were evaluated by scanning electron microscopy, x‐ray photoelectron spectroscopy, monofilament tensile test, and dynamic contact angle. Afterward, CF/epoxy composites were prepared, and their fracture morphology and interlaminar shear strength (ILSS) were examined. Results indicated that the TS sizing significantly increased the content of activated carbon on the surface of the CFs and improved the bonding effect between the fiber and the matrix. After TS was sized, the ILSS increased from 49.64 to 58.74 MPa, 18.34% higher than unsized CF/epoxy composites, showing the prominent interfacial reinforcement better than commercial Takemoto.

Qiu, Zhijie↗

DOE OSTI2015

Neighbor-directed histidine N(τ) alkylation. A route to imidazolium-containing phosphopeptide macrocycles

Our recently discovered, selective, on-resin route to N(τ)-alkylated imidazolium-containing histidine residues affords new strategies for peptide mimetic design. In this, we demonstrate the use of this chemistry to prepare a series of macrocyclic phosphopeptides, in which imidazolium groups serve as ring-forming junctions. These cationic moieties subsequently serve to charge-mask the phosphoamino acid group that directed their formation. Furthermore, neighbor-directed histidine N(τ)-alkylation opens the door to new families of phosphopeptidomimetics for use in a range of chemical biology contexts.

cationic dialkyl histidine↗