TY - JOUR A1 - Pisonero, J. A1 - Traub, Heike A1 - Cappella, Brunero A1 - Álvarez-Llamas, C. A1 - Méndez, A. A1 - Richter, Silke A1 - Ruiz Encinar, J. A1 - Costa-Fernandez, J. M. A1 - Bordel, N. T1 - Exploring quantitative cellular biomaging and assessment of CdSe/ZnS quantum dots cellular uptake in single cells, using ns-LA-ICP-SFMS N2 - High spatially resolved quantitative bioimaging of CdSe/ZnS Quantum Dots uptake in two kinds of cells is investigated combining laser ablation inductively coupled plasma mass spectrometry and the spatially resolved analysis of dried pL-droplets from a solution with a known concentration of Quantum Dots. Single cells and dried pL-droplets are morphologically characterized by Atomic Force Microscopy. A number concentration of CdSe/ZnS QDs between 3.5 104 and 48 104 is estimated to be uptaken by several selected single cells, after being incubated in the presence of a QDs suspension added to a standard cell culture medium. Mono-elemental bioimaging at subcellular resolution seems to show a higher number concentration of the CdSe/ZnS QDs in the cytosol around the cell nucleus. KW - LA-ICP-SFMS KW - Fast single pulse response KW - Quantitative bioimaging KW - Cellular uptake KW - HT22 KW - HeLa KW - Single cell KW - pL-droplets KW - CdSe/ZnS quantum Dots KW - AFM PY - 2021 DO - https://doi.org/10.1016/j.talanta.2021.122162 SN - 0039-9140 VL - 227 SP - 122162 PB - Elsevier B.V. AN - OPUS4-52121 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - CHAP A1 - Wolff, Dietmar A1 - Völzke, Holger A1 - Bevilacqua, A. A1 - Alejano, C. A1 - Conde, J.M. A1 - Einziger, R.E. A1 - Fukuda, S.-I. A1 - González Espartero, A. A1 - Gouzy-Portaix, S. A1 - Haddad Andalaf, R.E. A1 - Hambley, D. A1 - Issard, H. A1 - Kessler, J. A1 - Kurpaska, L. A1 - Legat, A. A1 - Qureshi, A.H. A1 - Ruiz, J. A1 - Shirai, K. A1 - Šmaižys, A. A1 - Verrastro, C.A. ED - González Espartero, A. T1 - Demonstrating performance of spent fuel and related storage system components during very long term storage - Final report of a coordinated research project N2 - This publication summarizes the work carried out during an IAEA coordinated research project (CRP) on safe and reliabe management of spent nuclear fuel. This work contributes to the overall goal of demonstrating the performance of spent nuclear fuel and related storage systems components over long durations, and facilitates the transfer of this knowledge to Member States. The technical areas addressed by the CRP participants were related to potential degradation mechanisms in metal casks and concrete overpacks, such as stress corrosion cracking; long term integrity and performance of the fuel cladding; thermo-mechanical behaviour of the metal seals; and long term gamma and neutron shielding capability. The participants also considered past and ongoing demonstration programmes. For each technical topic addressed the main conclusions have been drawn, including information on the development of specific monitoring and inspection techniques as well as future opportunities for closing relevant data gaps. A major achievement is also the establishment of a worldwide network of experts working on current research projects to demonstrate the long term performance of spent fuel in dry storage systems. KW - Spent fuel KW - Storage system components KW - Very long term storage PY - 2019 UR - https://www.iaea.org/publications/13553/demonstrating-performance-of-spent-fuel-and-related-storage-system-components-during-very-long-term-storage SN - 978–92–0–103319–2 SN - 1011–4289 VL - 1878 SP - 1 EP - 198 PB - IAEA Publishing Section CY - Vienna, Austria AN - OPUS4-48519 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - RPRT A1 - Maierhofer, Christiane A1 - Köpp, Christian A1 - Binda, L. A1 - Zanzi, L. A1 - Santiago, J.R. A1 - Knupfer, B. A1 - Johansson, B. A1 - Modena, C. A1 - da Porto, F. A1 - Marchisio, M. A1 - Gravina, F. A1 - Falci, M. A1 - Ruiz, J.C.G. A1 - Tomazevic, M. A1 - Bosiljkov, V. A1 - Hennen, C. A1 - Toledo, D.E.L. A1 - Zajc, A. A1 - delli Paoli, S. A1 - Drdácký, M. A1 - Válek, J. T1 - On-site investigation techniques for the structural evaluation of historic masonry buildings, Community research, Project Report EUR 21696 EN, Onsiteformasonry project KW - Non-destructive testing in civil engineering KW - Historic masonry KW - Damage KW - Cultural heritage KW - Complementary methods KW - Structural modelling KW - Guidelines and recommendations PY - 2006 SN - 92-894-9601-0 SP - 1 EP - 141 PB - Office for Official Publications of the European Communities CY - Luxembourg AN - OPUS4-14168 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Getenet, M. A1 - Garcia-Ruiz, J. M. A1 - Otálora, F. A1 - Emmerling, Franziska A1 - Al-Sabbagh, Dominik A1 - Verdugo-Escamilla, E. T1 - A comprehensive methodology for monitoring evaporitic mineral precipitation and hydrochemical evolution of saline lakes: The case of Lake Magadi soda brine (East African Rift Valley, Kenya) N2 - Lake Magadi, East African Rift Valley, is a hyperalkaline and saline soda lake highly enriched in Na+, K+, CO32–, Cl–, HCO3–, and SiO2 and depleted in Ca2+ and Mg2+, where thick evaporite deposits and siliceous sediments have been forming for 100 000 years. The hydrogeochemistry and the evaporite deposits of soda lakes are subjects of growing interest in paleoclimatology, astrobiology, and planetary sciences. In Lake Magadi, different hydrates of sodium carbonate/bicarbonate and other saline minerals precipitate. The precipitation sequence of these minerals is a key for understanding the hydrochemical evolution, the paleoenvironmental conditions of ancient evaporite deposits, and industrial crystallization. However, accurate determination of the precipitation sequence of these minerals was challenging due to the dependency of the different hydrates on temperature, water activity, pH and pCO2, which could induce phase transformation and secondary mineral precipitation during sample handling. Here, we report a comprehensive methodology applied for monitoring the evaporitic mineral precipitation and hydrochemical evolution of Lake Magadi. Evaporation and mineral precipitations were monitored by using in situ video microscopy and synchrotron X-ray diffraction of acoustically levitated droplets. The mineral patterns were characterized by ex situ Raman spectroscopy, X-ray diffraction, and scanning electron microscopy. Experiments were coupled with thermodynamic models to understand the evaporation and precipitation-driven hydrochemical evolution of brines. Our results closely reproduced the mineral assemblages, patterns, and textural relations observed in the natural setting. Alkaline earth carbonates and fluorite were predicted to precipitate first followed by siliceous sediments. Among the salts, dendritic and acicular trona precipitate first via fractional crystallization─reminiscent of grasslike trona layers of Lake Magadi. Halite/villiaumite, thermonatrite, and sylvite precipitate sequentially after trona from residual brines depleted in HCO3–. The precipitation of these minerals between trona crystals resembles the precipitation process observed in the interstitial brines of the trona layers. Thermonatrite precipitation began after trona equilibrated with the residual brines due to the absence of excess CO2 input. We have shown that evaporation and mineral precipitation are the major drivers for the formation of hyperalkaline, saline, and SiO2-rich brines. The discrepancy between predicted and actual sulfate and phosphate ion concentrations implies the biological cycling of these ions. The combination of different in situ and ex situ methods and modeling is key to understanding the mineral phases, precipitation sequences, and textural relations of modern and ancient evaporite deposits. The synergy of these methods could be applicable in industrial crystallization and natural brines to reconstruct the hydrogeochemical and hydroclimatic conditions of soda lakes, evaporite settings, and potentially soda oceans of early Earth and extraterrestrial planets. KW - Crystallization KW - Precipitation KW - Crystals KW - Evaporation KW - Minerals PY - 2022 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-546712 DO - https://doi.org/10.1021/acs.cgd.1c01391 SN - 1528-7483 VL - 22 IS - 4 SP - 2307 EP - 2317 PB - ACS Publications CY - Washington, DC AN - OPUS4-54671 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Menga, D. A1 - Low, J. L. A1 - Li, Y.-S. A1 - Arcon, I. A1 - Koyutürk, B. A1 - Wagner, F. A1 - Ruiz-Zepeda, F. A1 - Gaberscek, M. A1 - Paulus, B. A1 - Fellinger, Tim-Patrick T1 - Resolving the Dilemma of Fe-N-C Catalysts by the Selective Synthesis of Tetrapyrrolic Active Sites via an Imprinting Strategy N2 - Combining the abundance and inexpensiveness of their constituent elements with their atomic dispersion, atomically dispersed Fe−N−C catalysts represent the most promising alternative to precious-metal-based materials in proton Exchange membrane (PEM) fuel cells. Due to the high temperatures involved in their synthesis and the sensitivity of Fe ions toward carbothermal reduction, current synthetic methods are intrinsically limited in type and amount of the desired, catalytically active Fe−N4 sites, and high active site densities have been out of reach (dilemma of Fe−N−C catalysts). We herein identify a paradigm change in the synthesis of Fe−N−C catalysts arising from the developments of other M−N−C single-atom catalysts. Supported by DFT calculations we propose fundamental principles for the synthesis of M−N−C materials. We further exploit the proposed principles in a novel synthetic strategy to surpass the dilemma of Fe−N−C catalysts. The selective formation of tetrapyrrolic Zn−N4 sites in a tailor-made Zn−N−C material is utilized as an active-site imprint for the preparation of a corresponding Fe−N−C catalyst. By successive low- and high-temperature ion exchange reactions, we obtain a phase-pure Fe−N−C catalyst, with a high loading of atomically dispersed Fe (>3 wt %). Moreover, the catalyst is entirely composed of tetrapyrrolic Fe−N4 sites. The density of tetrapyrrolic Fe−N4 sites is more than six times as high as for previously reported tetrapyrrolic single-site Fe−N−C fuel cell catalysts. KW - Fe-N-C catalyst KW - Precious-group metal-free catalyst KW - Tetrapyrrolic active-site KW - Single-site catalyst KW - Fuel cell KW - Carbon materials PY - 2021 DO - https://doi.org/10.1021/jacs.1c04884 SN - 1520-5126 VL - 143 IS - 43 SP - 18010 EP - 18019 PB - American Chemical Society AN - OPUS4-53657 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Ruiz-Hervias, J. A1 - Simbruner, Kai A1 - Cristobal-Beneyto, M. A1 - Perez-Gallego, D. A1 - Zencker, Uwe T1 - Failure mechanisms in unirradiated ZIRLO® cladding with radial hydrides N2 - The purpose of this paper is to investigate the relationship between hydride morphology, in particular the presence of radial hydrides (RHs), stress state and failure mechanisms associated with the ring compression test (RCT). Samples of ZIRLO®cladding were pre-hydrided and subjected to thermo-mechanical treatments to precipitate long radial hydrides. The results show that the reorientation treatment was very successful. A considerable fraction of RHs was generated, the radial hydride continuity factor being around 80 to 90% of the wall thickness. The samples with reoriented hydrides were tested using the RCT at room temperature. Macroscopic brittle failure was observed with sudden load drops for displacements around 0.5 mm, with a calculated “offset strain”between 0.5 and 1%. Crack nucleation occurs in RHs located in regions with the highest values of hoop stress. These locations are the inner diameter of cladding at the vertical plane of the sample (12 and 6 o’clock positions) and the outer diameter at the horizontal plane (3 and 9 o’clock positions). Noticeable load drops in the RCT are associated with unstable crack propagation events through the radial hydride network, the crack front reaching up to 90% of the wall thickness in some cases. The failure micro-mechanism is quasi-cleavage in the hydrides and micro-void nucleation, growth and coalescence in the Zr matrix, with ductile tearing patches connecting neighboring hydrides. The main conclusion is that radial hydride metrics is not the only parameter that determines cladding failure in the presence of RHs, but the interaction between the location and continuity of RHs and the stress normal to the hydride (the hoop stress in this case). Consequently, if a radial hydride is located at a position within the cladding where the hoop stress is small, a crack will not be initiated easily in the RCT. KW - ZIRLO® KW - Cladding Embrittlement KW - Radial Hydrides KW - Failure Mechanism KW - Ring compression test PY - 2021 DO - https://doi.org/10.1016/j.jnucmat.2020.152668 SN - 0022-3115 VL - 544 SP - 152668 PB - Elsevier B.V. AN - OPUS4-52000 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Getenet, M. A1 - Otálora, F. A1 - Emmerling, Franziska A1 - Al-Sabbagh, Dominik A1 - García-Ruiz, J. M. T1 - Mineral precipitation and hydrochemical evolution through evaporitic processes in soda brines (East African Rift Valley) N2 - Soda lakes of the East African Rift Valley are hyperalkaline, hypersaline lakes extremely enriched in Na+, K+, Cl−, CO32−, HCO3−, and SiO2. In this paper, we investigate the chemical evolution in these lakes and the production of chemical sediments by salt precipitation via evaporation. Water samples from tributary springs and three lakes (Magadi, Nasikie Engida and Natron) have been experimentally studied by in-situ X-ray diffraction during evaporation experiments to characterize the sequence of mineral precipitation. These data are complemented by ex-situ diffraction studies, chemical analyses and thermodynamic hydrochemical calculations producing detailed information on the activity of all solution species and the saturation state of all minerals potentially generated by the given composition. Major minerals precipitating from these samples are sodium carbonates/bicarbonates as well as halite. The CO3/HCO3 ratio, controlled by pH, is the main factor defining the Na‑carbonates precipitation sequence: in lake brines where CO3/HCO3 > 1, trona precipitates first whereas in hot springs, where CO3/HCO3 ≪ 1, nahcolite precipitates instead of trona, which forms later via partial dissolution of nahcolite. Precipitation of nahcolite is possible only at lower pH values (pCO2 higher than −2.7) explaining the distribution of trona and nahcolite in current lakes and the stratigraphic sequences. Later, during evaporation, thermonatrite precipitates, normally at the same time as halite, at a very high pH (>11.2) after significant depletion of HCO3− due to trona precipitation. The precipitation of these soluble minerals increases the pH of the brine and is the main factor contributing to the hyperalkaline and hypersaline character of the lakes. Villiaumite, sylvite, alkaline earth carbonates, fluorapatite and silica are also predicted to precipitate, but most of them have not been observed in evaporation experiments, either because of the small amount of precipitates produced, kinetic effects delaying the nucleation of some phases, or by biologically induced effects in the lake chemistry that are not considered in our calculations. Even in these cases, the chemical composition in the corresponding ions allows for discussion on their accumulation and the eventual precipitation of these phases. The coupling of in-situ and ex-situ experiments and geochemical modelling is key to understanding the hydrogeochemical and hydroclimatic conditions of soda lakes, evaporite settings, and potentially soda oceans of early Earth and other extraterrestrial bodies. KW - Crystallization sequence KW - Hydrochemical evolution KW - Alkaline brines KW - Sodium carbonate minerals KW - Soda lakes KW - Evaporite deposits PY - 2023 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-568431 DO - https://doi.org/10.1016/j.chemgeo.2022.121222 SN - 0009-2541 VL - 616 SP - 1 EP - 13 PB - Elsevier CY - New York, NY AN - OPUS4-56843 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Sjöland, A. A1 - Christensen, P. A1 - Zetterström Evins, L. A1 - Bosbach, D. A1 - Duro, L. A1 - Farnan, I. A1 - Metz, V. A1 - Zencker, Uwe A1 - Ruiz-Hervias, J. A1 - Rodriguez-Villagra, N. A1 - Kiraly, M. A1 - Schillebeeckx, P. A1 - Rochman, D. A1 - Seidl, M. A1 - Dagan, R. A1 - Verwerft, M. A1 - Herranz Puebla, L. E. A1 - Hordynskyi, D. A1 - Feria, F. A1 - Vlassopoulos, E. T1 - Spent nuclear fuel management, characterisation, and dissolution behaviour: progress and achievement from SFC and DisCo N2 - SFC is a work package in Eurad that investigates issues related to the properties of the spent nuclear fuel in the back-end of the nuclear fuel cycle. Decay heat, nuclide inventory, and fuel integrity (mechanical and otherwise), and not least the related uncertainties, are among the primary focal points of SFC. These have very significant importance for the safety and operational aspect of the back-end. One consequence is the operation economy of the back-end, where deeper understanding and quantification allow for significant optimization, meaning that significant parts of the costs can be reduced. In this paper, SFC is described, and examples of results are presented at about half-time of the work package, which will finish in 2024. The DisCo project started in 2017 and finished in November 2021 and was funded under the Horizon 2020 Euratom program. It investigated if the properties of modern fuel types, namely doped fuel, and MOX, cause any significant difference in the dissolution behavior of the fuel matrix compared with standard fuels. Spent nuclear fuel experiments were complemented with studies on model materials as well as the development of models describing the solid state, the dissolution process, and reactive transport in the near field. This research has improved the understanding of processes occurring at the interface between spent nuclear fuel and aqueous solution, such as redox reactions. Overall, the results show that from a long-term fuel matrix dissolution point of view, there is no significant difference between MOX fuel, Cr+Al-doped fuel, and standard fuels. KW - Spent nuclear fuel management KW - Spent fuel characterization KW - Dissolution behaviour PY - 2023 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-572461 DO - https://doi.org/10.1051/epjn/2022029 SN - 2491-9292 VL - 9 SP - 1 EP - 12 PB - EDP Sciences CY - Les Ulis Cedex, France AN - OPUS4-57246 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Girard-Lauriault, Pierre-Luc A1 - Illgen, René A1 - Ruiz, J.-C. A1 - Wertheimer, M. R. A1 - Unger, Wolfgang T1 - Surface functionalization of graphite and carbon nanotubes by vacuum-ultraviolet photochemical reactions N2 - Graphite and multiwall carbon nanotube surfaces were functionalized by vacuum-ultraviolet induced photochemistry in NH3 or O2, in order to introduce amino- (NH2) or hydroxyl (OH) functionalities, respectively. Modified surfaces were characterized by X-ray photoelectron spectroscopy (XPS), which showed significant incorporation of nitrogen (N) and oxygen (O) at the materials’ surface. While high-resolution XP spectra did not yield much specific information about the incorporated functional groups, chemical derivatization with 4-trifluoromethyl benzaldehyde and trifluoroacetic anhydride accompanied by XPS enabled quantification of NH2 and OH groups, respectively. Using near edge X-ray absorption fine structure spectroscopy, we assessed the conservation of the aromatic structure following functionalization treatments. KW - Carbon nanotubes KW - Graphite KW - Vacuum ultraviolet photochemistry KW - Surface functionalization KW - Amino groups KW - Hydroxyl KW - Derivatization PY - 2012 DO - https://doi.org/10.1016/j.apsusc.2012.03.012 SN - 0169-4332 SN - 1873-5584 VL - 258 IS - 22 SP - 8448 EP - 8454 PB - North-Holland CY - Amsterdam AN - OPUS4-26233 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Girard-Lauriault, Pierre-Luc A1 - Ruiz, J.-C. A1 - Gross, Thomas A1 - Wertheimer, M. R. A1 - Unger, Wolfgang T1 - Ultra-shallow chemical characterization of organic thin films deposited by plasma and vacuum-ultraviolet, using angle- and excitation energy-resolved XPS N2 - Nitrogen (N)-rich organic thin films were deposited using both low-pressure plasma- and vacuum-ultraviolet-based techniques, from mixtures of ammonia (NH3) and ethylene (C2H4). These films were investigated using angle-resolved and excitation energy resolved X-ray photoelectron spectroscopy (ARXPS and ERXPS, respectively) in order to determine their sub-surface chemical profiles. These two techniques enable one to tune the “XPS 95%” information depth, z 95%, by varying either the angle or the excitation energy. Using a combination of both techniques, z 95% can be varied continuously from 0.7 to 11 nm. The surface-near chemistry is investigated using both high-resolution C 1s spectra and elemental concentrations derived from elemental peak intensities. Results show that while laboratory XPS, and even ARXPS, suggest homogenous surface chemistries, the novel combination of ARXPS and ERXPS points to the existence of a compositional profile in the extreme outer surface layer. Our conclusions are supported by simulations using SESSA software. KW - Plasma polymers KW - Vacuum ultraviolet photopolymers KW - Synchrotron XPS KW - Depth profile PY - 2011 DO - https://doi.org/10.1007/s11090-011-9306-3 SN - 0272-4324 VL - 31 IS - 4 SP - 535 EP - 550 PB - Plenum Publ. Corp. CY - New York, NY, USA AN - OPUS4-23993 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER -