Publications

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For long-term storage, spent nuclear fuel (SNF) is placed in dry storage systems, commonly consisting of welded stainless steel canisters enclosed in ventilated overpacks. Choride-induced stress corrosion cracking (CISCC) of these canisters may occur due to the deliquescence of sea-salt aerosols as the canisters cool. Current experimental and modeling efforts to evaluate canister CISCC assume that the deliquescent brines, once formed, persist on the metal surface, without changing chemical or physical properties. Here we present data that show that magnesium chloride rich-brines, which form first as the canisters cool and sea-salts deliquesce, are not stable at elevated temperatures, degassing HCl and converting to solid carbonates and hydroxychloride phases, thus limiting conditions for corrosion. Moreover, once pitting corrosion begins on the metal surface, oxygen reduction in the cathode region surrounding the pits produces hydroxide ions, increasing the pH under some experimental conditions, leads to precipitation of magnesium hydroxychloride hydrates. Because magnesium carbonates and hydroxychloride hydrates are less deliquescent than magnesium chloride, precipitation of these compounds causes a reduction in the brine volume on the metal surface, potentially limiting the extent of corrosion. If taken to completion, such reactions may lead to brine dry-out, and cessation of corrosion.

Photovoltaic (PV) power plants and their constituent components, by virtue of their application, are exposed to some of the harshest outdoor terrestrial environments. Most equipment is subject directly to the environment and myriad stresses (micro and macro environment). Other aspects including local site conditions, construction variability and quality, and maintenance practices also influence the likelihood of such hazards. Many discrete components, including PV modules, wires, connectors, wire management devices, combiner boxes, protection devices, inverters, and transformers, make up the PV generation system. While there are abundant data that illustrate PV modules and PV inverters to be the major contributors of PV system failures, the mentioned data illustrate the importance of minimizing failures in the often ignored components such as PV connectors, PV wires (both above and below ground), wire splices, fuses, fuse holders, fuse holder enclosures, and wire management devices. With the exception of PV fuses, these components predominantly use polymeric materials. Therefore, it is crucial to understand the typical materials used in components, degradation processes and mechanisms leading to component failure, and their impact on system performance or failure. It further provides some practical considerations, approaches, and methods in addressing the problems with practical solutions in the design to assure the performance of the PV plant over the intended design lifetime.

This progress report describes work done in FY18 at Sandia National Laboratories (SNL) to assess the localized corrosion performance of container/cask materials used in the interim storage of spent nuclear fuel (SNF). The work focuses on stress corrosion cracking (SCC), the only mechanism by which a through-wall crack could potentially form in a canister outer wall over time intervals that are shorter than possible dry storage times. Work in FY18 continued several studies initiated in FY17 that are aimed at refining the understanding of the chemical and physical environment on canister surfaces, and evaluating the relationship between chemical and physical environment and the form and extent of corrosion that occurs. The SNL canister environment work focused on evaluating the stability of sea-salt deliquescent brines on the heated canister surface; an additional opportunity to analyze dusts sampled from an inservice spent nuclear fuel storage canister also arose. The SNL corrosion work focused predominantly on pitting corrosion, a necessary precursor for SCC, and process of pit-to-crack transition. SNL is collaborating with several university partners to investigate SCC crack growth experimentally, providing guidance for design and interpretation of experiments. The scope of these efforts targets near-marine Independent Spent Fuel Storage Installation environments which are generally considered to be most aggressive for pitting and SCC. Work to define the chemical and physical environment that could develop on storage canister surfaces in near-marine environments included experiments to evaluate the thermal stability of magnesium chloride brines, representative of the first brines to form when sea-salts deliquesce, with the specific goal of understanding and interpreting results of sea-salt and magnesium chloride corrosion experiments carried out under accelerated conditions. The experiments showed that magnesium chloride brines, and by extension, low RH sea-salt deliquescent brines, are not stable at elevated temperatures, losing chloride via degassing of HC1 and conversion to Mg-hydroxychlorides and carbonates. The experiments were carried out on an inert substrate to eliminate the effects of corrosion reactions, simulating brine stabilities in the absence of, or prior to, corrosion. Moreover, analysis of salts recovered from actively corroding metal samples shows that corrosion also supports or drives conversion of magnesium chloride or sea-salt brines to less deliquescent salts. This process has significant implications on corrosion, as the secondary phases are less deliquescent than magnesium chloride; the conversion reaction results in decreases in brine volume, and potentially results in brine dry-out. The deliquescence properties of these reaction products will be a topic of active research in FY19.

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Stress corrosion cracks (SCC) represent a major concern for the structural integrity of engineered metal structures. In hazardous or restricted-access environments, remote detection of corrosion or SCC frequently relies on visual methods; however, with standard VT-1 visual inspection techniques, probabilities of SCC detection are low. Here, we develop and evaluate an improved optical sensor for SCC in restricted access-environments by combining a robotically controlled camera/fiber-optic based probe with software-based super-resolution imaging (SRI) techniques to increase image quality and detection of SCC. SRI techniques combine multiple images taken at different viewing angles, locations, or rotations, to produce a single higher- resolution composite image. We have created and tested an imaging system and algorithms for combining optimized, controlled camera movements and super- resolution imaging, improving SCC detection probabilities, and potentially revolutionizing techniques for remote visual inspections of any type.

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Metals across all industries demand anticorrosion surface treatments and drive a continual need for high-performing and low-cost coatings. Here we demonstrate polymer-clay nanocomposite thin films as a new class of transparent conformal barrier coatings for protection in corrosive atmospheres. Films assembled via layer-by-layer deposition, as thin as 90 nm, are shown to reduce copper corrosion rates by >1000× in an aggressive H2S atmosphere. These multilayer nanobrick wall coatings hold promise as high-performing anticorrosion treatment alternatives to costlier, more toxic, and less scalable thin films, such as graphene, hexavalent chromium, or atomic-layer-deposited metal oxides.

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This study describes the evolving state of electrolyte and corrosion processes associated with sodium chloride on copper at the initial stage of corrosion and the critical implications of this behavior on controlling kinetics and damage distributions. Sodium chloride droplets were placed on copper in humid conditions and the resulting electrolyte properties, corrosion products and damage were characterized over time using time-lapse imaging, micro Raman spectroscopy, TOF-SIMS and optical profilometry. Within minutes of NaCl droplet placement, NaOH-rich films resultant from oxygen reduction advanced stepwise from the droplets, leaving behind concentric trenching attack patterns suggestive of moving anode-cathode pairs at the alkaline film front. Corrosion attack under these spreading alkaline films was up to 10x greater than under the original NaCl drops. Furthermore, solid Cu2Cl(OH)3 shells formed over the surface of the NaCl drops within hours of exposure. Thermodynamic modeling along with immersed electrochemical experiments in simulated droplet and films electrolytes were used to rationalize this behavior and build a description of the rapidly evolving corroding system.

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For long-term dry storage, most spent nuclear fuel in the United States is placed in welded 304 SS or 316 SS canisters that are stored within passively ventilated overpacks. As the canisters cool, sea-salt aerosols deposited on the canister surfaces will deliquesce to form potentially corrosive brines. We have used thermodynamic modeling to predict the chemical composition of the brines that form by deliquescence of sea-salt aerosols, and to estimate brine volumes and salt/brine volume ratios as a function of temperature and atmospheric relative humidity. We have also mixed representative brines and measured the physical and chemical properties of those brines over a range of temperatures. These data provide a matrix that can be used to predict the evolution of deliquescent brine properties over time on storage canister surfaces, as the canisters cool and surface relative humidity increases. Brine volumes and properties affect corrosion kinetics and damage distributions on the metal surface, and may offer important constraints on the expected rate and extent of corrosion and the timing of SCC crack initiation. The predicted brines do not consider reactions with atmospheric gases that are known to affect sea-salt particle and deliquescent brine compositions under field conditions. The potential effects of such reactions are discussed, and preliminary modeling and experimental data are presented.

The corrosion behavior of selective laser melted (SLM) 304L was investigated and compared to conventional wrought 304L in aqueous chloride and acidic solutions. Through immersed electrochemical testing and exposure in acidic solutions, the SLM 304L exhibited superior pitting resistance in the polished state compared to wrought 304L. However, the surface condition of the SLM material had a great impact on its corrosion resistance, with the grit-blasted condition exhibiting severely diminished pitting resistance. Local scale, capillary micro-electrochemical and scanning electrochemical microscopy investigations, identified porosity as a contributing factor to decreased corrosion resistance. Preferential corrosion attack was not observed to be related to the characteristic underlying cellular microstructure produced through SLM processing. This study highlights the effects of SLM microstructural features on corrosion resistance, specifically the substantial influence of surface finish on SLM corrosion behavior and the need for development and optimization of processing techniques to improve surface finish.

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In June 2017, dust and salt samples were collected from the surface of Spent Nuclear Fuel (SNF) dry storage canisters at the Calvert Cliffs Nuclear Power Plant. The samples were delivered to Sandia National laboratories for analysis. Two types of samples were collected: filter-backed Scotch-Brite TM pads were used to collect dry dust samples for characterization of salt and dust morphologies and distributions; and Saltsmart TM test strips were used to collect soluble salts for determining salt surface loadings per unit area. After collection, the samples were sealed into plastic sleeves for shipping. Condensation within the sleeves containing the Scotch-Brite TM samples remobilized the salts, rendering them ineffective for the intended purpose, and also led to mold growth, further compromising the samples; for these reasons, the samples were not analyzed. The SaltSmart TM samples were unaffected and were analyzed by ion chromatography for major anions and cations. The results of those analyses are presented here.

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This progress report describes work done in FY17 at Sandia National Laboratories (SNL) to assess the localized corrosion performance of container/cask materials used in the interim storage of spent nuclear fuel (SNF). Of particular concern is stress corrosion cracking (SCC), by which a through-wall crack could potentially form in a canister outer wall over time intervals that are shorter than possible dry storage times. Work in FY17 refined our understanding of the chemical and physical environment on canister surfaces, and evaluated the relationship between chemical and physical environment and the form and extent of corrosion that occurs. The SNL corrosion work focused predominantly on pitting corrosion, a necessary precursor for SCC, and process of pit-to-crack transition; it has been carried out in collaboration with university partners. SNL is collaborating with several university partners to investigate SCC crack growth experimentally, providing guidance for design and interpretation of experiments.

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The corrosion susceptibility of a laser powder bed fusion (LPBF) additively manufactured alloy, UNS S17400 (17-4 PH), was explored compared to conventional wrought material. Microstructural characteristics were characterized and related to corrosion behavior in quiescent, aqueous 0.6 M NaCl solutions. Electrochemical measurements demonstrated that the LPBF 17-4 PH alloy exhibited a reduced passivity range and active corrosion compared to its conventional wrought counterpart. A microelectrochemical cell was used to further understand the effects of the local scale and attributed the reduced corrosion resistance of the LPBF material to pores with diameters ≥50 μm.

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Metal additive manufacturing (AM) has recently become a desirable process for complex parts across a broad range of applications. However, AM materials often have a varied microstructure due to non-equilibrium solidification conditions. While some adjustments have been made in manufacturing to enhance mechanical traits, very little attention has been directed at understanding the corrosion properties of these materials. The microstructural characteristics of the AM materials may lead to reduction in the corrosion resistance of the AM alloys compared to their conventional counterparts. This presentation explores the corrosion susceptibility of AM stainless steels in aqueous sodium chloride environments as well as industry relevant solutions. Further detailed corrosion studies combined with microstructural characterization provide insight into the microstructural influences on corrosion.

Corrosion of aluminum and aluminum alloys under atmospheric exposure has been well documented for outdoor conditions. While these studies expose the effects of environmental severity they do not explicitly establish the dependence of corrosion rate on salt loading. Accelerated laboratory studies have shown that initial corrosion rates are generally higher with higher salt loadings, but, over time corrosion appears to effectively stifle for low loadings of NaCl (<100 μg/cm2) under fixed humidity conditions. This has previously been attributed to the stability or passivation of the surface that is pH and, in turn, CO2 dependent. Another possible explanation could be the gettering of NaCl by corrosion product leading to surface drying and depletion of the corrosion aggressor. This paper explores the effects of selected NaCl loading densities vs. exposure time of UNS A91100 at both the macro and micro scale to illuminate the possible mechanisms leading to corrosion stifling. Through this work, an understanding of the relationship between corrosion in atmospheric systems versus the variation of a specific environmental severity factor, NaCl loading density, will be further developed.

While arc-faults are rare in electrical installations, many documented events have led to fires that resulted in significant damage to energy-generation, commercial and residential systems, as well as surrounding structures, in both the United States and abroad. Arc-plasma discharges arise over time due to a variety of reliability issues related to cable material degradation, electrical and mechanical stresses or acute conductive wiring dislocations. These may lead to discontinuity between energized conductors, facilitating arcing events and fires. Arc-flash events rapidly release significant energy in a localized volume, where the electric arc experiences a reduction in resistance. This facilitates a reduction in electrical resistance as the arc temperature and pressure can increase rapidly. Strong pressure waves, electromagnetic interference (EMI), and intense light from an arc pose a threat to electrical worker safety and system equipment. This arc-fault primer provides basic fundamental insight into arc-fault plasma discharges, and an overview of direct current (DC) and alternating current (AC) arc-fault phenomena. This primer also covers pressure waves and EMI arc-fault hazard analyses related to incident energy prediction and potential damage analysis. Mitigation strategies are also discussed related to engineering design and employment of protective devices including arc-fault circuit interrupters (AFCIs). Best practices related to worker safety are also covered, especially as they pertain to electrical codes and standards, particularly Institute of Electrical and Electronics Engineers (IEEE) 1584 and National Fire Protection Agency (NFPA) 70E. Throughout the primer various modelling and test capabilities at Sandia National Laboratories are also covered, especially as they relate to novel methods of arc-fault/arc-flash characterization and mitigation approaches. Herein, this work describes methods for producing and characterizing controlled, sustained arcs at atmospheric pressures as well as methods for mitigation with novel materials.

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During routine pharmaceutical development and scale-up work, severe corrosion of a Hastelloy Alloy C-22 (Alloy 22) filter dryer was observed after single, short (several hour) contact with the product slurry at room temperature. Initial investigations showed that the presence of both 2,3-dichloro-5,6-dicyano-1,4-benzoquinone (DDQ) and HCl was sufficient in an acetonitrile solution to cause rapid corrosion of Alloy 22. More detailed mass loss studies showed initial corrosion rates exceeding 25 mm/y that then decreased over several hours to steady state rates of 3 mm/y to 5 mm/y. The corrosion was highly uniform. Electrochemical measurements demonstrated that although Alloy 22 is spontaneously passive in acetonitrile solution, the presence of HCl leads to the development of a transpassive region. DDQ is a sufficiently strong oxidizer, particularly in acidic solutions, to polarize the Alloy 22 well into the transpassive region, leading to the observed highcorrosion rates.

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Three balance of systems (BOS) connector designs common to industry were investigated as a means of assessing reliability from the perspective of arc fault risk. These connectors were aged in field and laboratory environments and performance data captured for future development of a reliability model. Comparison of connector resistance measured during damp heat, mixed flowing gas and field exposure in a light industrial environment indicated disparities in performance across the three designs. Performance was, in part, linked to materials of construction. A procedure was developed to evaluate new and aged connectors for arc fault risk and tested for one of the designs. Those connectors exposed to mixed flowing gas corrosion exhibited considerable Joule heating that may enhance arcing behavior, suggesting temperature monitoring as a potential method for arc fault prognostics. These findings, together with further characterization of connector aging, can provide operators of photovoltaic installations the information necessary to develop a data-driven approach to BOS connector maintenance as well as opportunities for arc fault prognostics.

The continued exponential growth of photovoltaic technologies paves a path to a solar-powered world, but requires continued progress toward low-cost, high-reliability, high-performance photovoltaic (PV) systems. High reliability is an essential element in achieving low-cost solar electricity by reducing operation and maintenance (O&M) costs and extending system lifetime and availability, but these attributes are difficult to verify at the time of installation. Utilities, financiers, homeowners, and planners are demanding this information in order to evaluate their financial risk as a prerequisite to large investments. Reliability research and development (R&D) is needed to build market confidence by improving product reliability and by improving predictions of system availability, O&M cost, and lifetime. This project is focused on understanding, predicting, and improving the reliability of PV systems. The two areas being pursued include PV arc-fault and ground fault issues, and inverter reliability.

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