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- ItemDynamic Light Scattering on Nanoparticles in Microgravity in a Drop Tower(Heidelberg : Springer, 2022) Pyttlik, Andrea; Kuttich, Björn; Kraus, TobiasGravity affects colloidal dispersions via sedimentation and convection. We used dynamic light scattering (DLS) to quantify the mobility of nanoparticles on ground and in microgravity. A DLS instrument was adapted to withstand the accelerations in a drop tower, and a liquid handling set-up was connected in order to stabilize the liquid temperature and enable rapid cooling or heating. Light scattering experiments were performed in the drop tower at ZARM (Bremen, Germany) during a microgravity interval of 9.1 s and compared to measurements on ground. Particle dynamics were analyzed at constant temperature and after a rapid temperature drop using a series of DLS measurements with 1 s integration time. We observed nanoparticles with average gold core diameters of 7.8 nm and non-polar oleylamine shells that were dispersed in tetradecane and had an average hydrodynamic diameter of 21 nm. The particles did not change their diameter in the observed temperature range. The particle dynamics inferred from DLS on ground and in microgravity were in good agreement, demonstrating the possibility to perform reliable DLS measurements in a drop tower.
- ItemInterlaboratory study assessing the analysis of supercapacitor electrochemistry data(New York, NY [u.a.] : Elsevier, 2023) Gittins, Jamie W.; Chen, Yuan; Arnold, Stefanie; Augustyn, Veronica; Balducci, Andrea; Brousse, Thierry; Frackowiak, Elzbieta; Gómez-Romero, Pedro; Kanwade, Archana; Köps, Lukas; Jha, Plawan Kumar; Lyu, Dongxun; Meo, Michele; Pandey, Deepak; Pang, Le; Presser, Volker; Rapisarda, Mario; Rueda-García, Daniel; Saeed, Saeed; Shirage, Parasharam M.; Ślesiński, Adam; Soavi, Francesca; Thomas, Jayan; Titirici, Maria-Magdalena; Wang, Hongxia; Xu, Zhen; Yu, Aiping; Zhang, Maiwen; Forse, Alexander C.Supercapacitors are fast-charging energy storage devices of great importance for developing robust and climate-friendly energy infrastructures for the future. Research in this field has seen rapid growth in recent years, therefore consistent reporting practices must be implemented to enable reliable comparison of device performance. Although several studies have highlighted the best practices for analysing and reporting data from such energy storage devices, there is yet to be an empirical study investigating whether researchers in the field are correctly implementing these recommendations, and which assesses the variation in reporting between different laboratories. Here we address this deficit by carrying out the first interlaboratory study of the analysis of supercapacitor electrochemistry data. We find that the use of incorrect formulae and researchers having different interpretations of key terminologies are major causes of variability in data reporting. Furthermore we highlight the more significant variation in reported results for electrochemical profiles showing non-ideal capacitive behaviour. From the insights gained through this study, we make additional recommendations to the community to help ensure consistent reporting of performance metrics moving forward.
- ItemCracking and associated volumetric expansion of NMC811 secondary particles(New York, NY [u.a.] : Elsevier, 2023) Shishvan, S.S.; Fleck, N.A.; McMeeking, R.M.; Deshpande, V.S.Secondary particles comprising a large number of nickel-rich single crystal primary particles are extensively used as storage particles in cathodes of lithium-ion batteries. It is well-established that crack formation in secondary particles is an important degradation mode that contributes to decline in battery performance. Recent X-ray tomographic observations suggest that, at very low C-rates, concentration gradients of lithium within an NMC811 secondary particle are negligible yet cracking still occurs. Additionally, during delithiation the primary particles shrink yet a volumetric expansion of the secondary particle occurs. These observations are explained by a numerical model of distributed cracking due to the extreme anisotropy of lithiation strain of primary particles. The incompatible deformation from grain to grain induces large self-stresses even in the absence of spatial gradients in the lithium concentration. The stress state is sufficient to drive a dynamic catastrophic fracture event, and the associated kinetic energy acquired by the primary particles moves them apart (akin to an explosive event) with the carbon and binder domain surrounding each secondary particle restricting the outward motion of the primary particles. It is predicted that a volume expansion of the secondary particles on the order of 20 % accompanies cracking, in agreement with recently reported observations.
- ItemRhodamine 6G and 800 intermolecular heteroaggregates embedded in PMMA for near-infrared wavelength shifting(London [u.a.] : RSC, 2022) Castillo-Seoane, Javier; Gonzalez-Garcia, Lola; Obrero-Perez, José M.; Aparicio, Francisco J.; Borrás, Ana; González-Elipe, Agustín R.; Barranco, Ángel; Sanchez-Valencia, Juan R.The opto-electronic properties of small-molecules and functional dyes usually differ when incorporated into solid matrices with respect to their isolated form due to an aggregation phenomenon that alters their optical and fluorescent properties. These spectroscopic modifications are studied in the framework of the exciton theory of aggregates, which has been extensively applied in the literature for the study of molecular aggregates of the same type of molecules (homoaggregation). Despite the demonstrated potential of the control of the heteroaggregation process (aggregation of different types of molecules), most of the reported works are devoted to intramolecular aggregates, complex molecules formed by several chromophores attached by organic linkers. The intramolecular aggregates are specifically designed to hold a certain molecular structure that, on the basis of the exciton theory, modifies their optical and fluorescent properties with respect to the isolated chromophores that form the molecule. The present article describes in detail the incorporation of Rhodamine 6G (Rh6G) and 800 (Rh800) into polymeric matrices of poly-(methyl methacrylate), PMMA. The simultaneous incorporation of both dyes results in an enhanced fluorescent emission in the near-infrared (NIR), originating from the formation of ground-state Rh6G–Rh800 intermolecular heteroaggregates. The systematic control of the concentration of both rhodamines provides a model system for the elucidation of the heteroaggregate formation. The efficient energy transfer between Rh6G and Rh800 molecules can be used as wavelength shifters to convert effectively the light from visible to NIR, a very convenient wavelength range for many practical applications which make use of inexpensive commercial detectors and systems.
- ItemToward a Li-Ion Battery Ontology Covering Production and Material Structure(Weinheim [u.a.] : Wiley-VCH, 2022) Mutz, Marcel; Perovic, Milena; Gümbel, Philip; Steinbauer, Veit; Taranovskyy, Andriy; Li, Yunjie; Beran, Lisa; Käfer, Tobias; Dröder, Klaus; Knoblauch, Volker; Kwade, Arno; Presser, Volker; Werth, Dirk; Kraus, TobiasAn ontology for the structured storage, retrieval, and analysis of data on lithium-ion battery materials and electrode-to-cell production is presented. It provides a logical structure that is mapped onto a digital architecture and used to visualize, correlate, and make predictions in battery production, research, and development. Materials and processes are specified using a predetermined terminology; a chain of unit processes (steps) connects raw materials and products (items) of battery cell production. The ontology enables the attachment of analytical methods (characterization methods) to items. Workshops and interviews with experts in battery materials and production processes are conducted to ensure that the structure is conformable both for industrial-scale and laboratory-scale data generation and implementation. Raw materials and intermediate products are identified and defined for all steps to the final battery cell. Steps and items are defined based on current standard materials and process chains using terms that are in common use. Alternative structures and the connection of the ontology to other existing ontologies are discussed. The contribution provides a pragmatic, accessible way to unify the storage of materials-oriented lithium-ion battery production data. It aids the linkage of such data with domain knowledge and the automation of data analysis in production and research.
- ItemOn the adhesion between thin sheets and randomly rough surfaces(Lausanne : Frontiers Media, 2022) Wang , Anle; Müser, Martin H.Thin, elastic sheets are well known to adapt to rough counterfaces, whereby adhesive interactions and pull-off stresses σp can be significant, yet no generally applicable, quantitative guideline has been suggested hitherto as to when a sheet should be considered thin enough to be sticky. Using computer simulations, we find that the dependence of σp on surface energy γ has a high and a low-pull-off-stress regime. For randomly rough surfaces, we locate the dividing line at the point, where γ is approximately half the elastic energy per unit area needed to make conformal contact, which is the same ratio as for semi-infinite elastic solids. This rule of thumb also applies to a certain degree for single-wavelength roughness, in which case the transition from low to high stickiness occurs when at the moment of maximum tension contact is not only broken at the height maxima but also at the saddle points.
- ItemAdvancing environmental intelligence through novel approaches in soft bioinspired robotics and allied technologies: I-Seed project position paper for Environmental Intelligence in Europe(New York,NY,United States : Association for Computing Machinery, 2022) Mazzolai, Barbara; Kraus, Tobias; Pirrone, Nicola; Kooistra, Lammert; De Simone, Antonio; Cottin, Antoine; Margheri, LauraThe EU-funded FET Proactive Environmental Intelligence project "I-Seed"(Grant Agreement n. 101017940, https://www.iseedproject.eu/) targets towards the development of a radically simplified and environmentally friendly approach for environmental monitoring. Specifically, I-Seed aims at developing a new generation of self-deployable and biodegradable soft miniaturized robots, inspired by the morphology and dispersion abilities of plant seeds, able to perform low-cost, environmentally responsible, in-situ measurements. The natural functional mechanisms of seeds dispersal offer a rich source of robust, highly adaptive, mass and energy efficient mechanisms, and behavioral and morphological intelligence, which can be selected and implemented for advanced, but simple, technological inventions. I-Seed robots are conceived as unique in their movement abilities because inspired by passive mechanisms and materials of natural seeds, and unique in their environmentally friendly design because made of all biodegradable components. Sensing is based on a chemical transduction mechanism in a stimulus-responsive sensor material with fluorescence-based optical readout, which can be read via one or more drones equipped with fluorescent LiDAR technology and a software able to perform a real time georeferencing of data. The I-Seed robotic ecosystem is envisioned to be used for collecting environmental data in-situ with high spatial and temporal resolution across large remote areas where no monitoring data are available, and thus for extending current environmental sensor frameworks and data analysis systems.
- ItemRelationship between corrosion and nanoscale friction on a metallic glass(Frankfurt, M. : Beilstein-Institut zur Förderung der Chemischen Wissenschaften, 2022) Ma, Haoran; Bennewitz, RolandMetallic glasses are promising materials for microdevices, although corrosion and friction limit their effectiveness and durability. We investigated nanoscale friction on a metallic glass in corrosive solutions after different periods of immersion time using atomic force microscopy to elucidate the influence of corrosion on nanoscale friction. The evolution of friction upon repeated scanning cycles on the corroded surfaces reveals a bilayer surface oxide film, of which the outer layer is removed by the scanning tip. The measurement of friction and adhesion allows one to compare the physicochemical processes of surface dissolution at the interface of the two layers. The findings contribute to the understanding of mechanical contacts with metallic glasses under corrosive conditions by exploring the interrelation of microscopic corrosion mechanisms and nanoscale friction.
- ItemDegradation analysis of tribologically loaded carbon nanotubes and carbon onions([London] : Macmillan Publishers Limited, 2023) MacLucas, T.; Grützmacher, P.; Husmann, S.; Schmauch, J.; Keskin, S.; Suarez, S.; Presser, V.; Gachot, C.; Mücklich, F.Coating laser-patterned stainless-steel surfaces with carbon nanotubes (CNT) or carbon onions (CO) forms a tribological system that provides effective solid lubrication. Lubricant retention represents the fundamental mechanism of this system, as storing the particles inside the pattern prevents lubricant depletion in the contact area. In previous works, we used direct laser interference patterning to create line patterns with three different structural depths on AISI 304 stainless-steel platelets. Electrophoretic deposition subsequently coated the patterned surfaces with either CNTs or COs. Ball-on-disc friction tests were conducted to study the effect of structural depth on the solid lubricity of as-described surfaces. The results demonstrated that the shallower the textures, the lower the coefficient of friction, regardless of the applied particle type. This follow-up study examines the carbon nanoparticles’ structural degradation after friction testing on substrates patterned with different structural depths (0.24, 0.36, and 0.77 µm). Raman characterization shows severe degradation of both particle types and is used to classify their degradation state within Ferrari’s three-stage amorphization model. It was further shown that improving CNT lubricity translates into increasing particle defectivity. This is confirmed by electron microscopy, which shows decreasing crystalline domains. Compared to CNTs, CO-derived tribofilms show even more substantial structural degradation.
- ItemDual-Use of Seawater Batteries for Energy Storage and Water Desalination(Weinheim : Wiley-VCH, 2022) Arnold, Stefanie; Wang, Lei; Presser, VolkerSeawater batteries are unique energy storage systems for sustainable renewable energy storage by directly utilizing seawater as a source for converting electrical energy and chemical energy. This technology is a sustainable and cost-effective alternative to lithium-ion batteries, benefitting from seawater-abundant sodium as the charge-transfer ions. Research has significantly improved and revised the performance of this type of battery over the last few years. However, fundamental limitations of the technology remain to be overcome in future studies to make this method even more viable. Disadvantages include degradation of the anode materials or limited membrane stability in aqueous saltwater resulting in low electrochemical performance and low Coulombic efficiency. The use of seawater batteries exceeds the application for energy storage. The electrochemical immobilization of ions intrinsic to the operation of seawater batteries is also an effective mechanism for direct seawater desalination. The high charge/discharge efficiency and energy recovery make seawater batteries an attractive water remediation technology. Here, the seawater battery components and the parameters used to evaluate their energy storage and water desalination performances are reviewed. Approaches to overcoming stability issues and low voltage efficiency are also introduced. Finally, an overview of potential applications, particularly in desalination technology, is provided.