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End date: 2022 × Start date: 2022 × End date: 2022 × Start date: 2022 × DDC: 600 ×

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    High-Quality Graphene Using Boudouard Reaction
    (Weinheim : Wiley-VCH, 2022) Grebenko, Artem K.; Krasnikov, Dmitry V.; Bubis, Anton V.; Stolyarov, Vasily S.; Vyalikh, Denis V.; Makarova, Anna A.; Fedorov, Alexander; Aitkulova, Aisuluu; Alekseeva, Alena A.; Gilshtein, Evgeniia; Bedran, Zakhar; Shmakov, Alexander N.; Alyabyeva, Liudmila; Mozhchil, Rais N.; Ionov, Andrey M.; Gorshunov, Boris P.; Laasonen, Kari; Podzorov, Vitaly; Nasibulin, Albert G.
    Following the game-changing high-pressure CO (HiPco) process that established the first facile route toward large-scale production of single-walled carbon nanotubes, CO synthesis of cm-sized graphene crystals of ultra-high purity grown during tens of minutes is proposed. The Boudouard reaction serves for the first time to produce individual monolayer structures on the surface of a metal catalyst, thereby providing a chemical vapor deposition technique free from molecular and atomic hydrogen as well as vacuum conditions. This approach facilitates inhibition of the graphene nucleation from the CO/CO2 mixture and maintains a high growth rate of graphene seeds reaching large-scale monocrystals. Unique features of the Boudouard reaction coupled with CO-driven catalyst engineering ensure not only suppression of the second layer growth but also provide a simple and reliable technique for surface cleaning. Aside from being a novel carbon source, carbon monoxide ensures peculiar modification of catalyst and in general opens avenues for breakthrough graphene-catalyst composite production.
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    Tailoring Intermolecular Interactions Towards High‐Performance Thermoelectric Ionogels at Low Humidity
    (Weinheim : Wiley-VCH, 2022) Zhao, Wei; Sun, Tingting; Zheng, Yiwei; Zhang, Qihao; Huang, Aibin; Wang, Lianjun; Jiang, Wan
    Development of ionic thermoelectric (iTE) materials is of immense interest for efficient heat-to-electricity conversion due to their giant ionic Seebeck coefficient (Si), but challenges remain in terms of relatively small Si at low humidity, poor stretchability, and ambiguous interaction mechanism in ionogels. Herein, a novel ionogel is reported consisting of polyethylene oxide (PEO), polyethylene oxide-polypropylene oxide-polyethylene oxide (P123), and 1-ethyl-3-methylimidazolium acetate (Emim:OAC). By delicately designing the interactions between ions and polymers, the migration of anions is restricted due to their strong binding with the hydroxyl groups of polymers, while the transport of cations is facilitated through segmental motions due to the increased amorphous regions, thereby leading to enlarged diffusion difference between the cations and anions. Moreover, the plasticizing effect of P123 and Emim:OAC can increase the elongation at break. As a consequence, the ionogel exhibits excellent properties including high Si (18 mV K−1 at relative humidity of 60%), good ionic conductivity (1.1 mS cm−1), superior stretchability (787%), and high stability (over 80% retention after 600 h). These findings show a promising strategy to obtain multifunctional iTE materials by engineering the intermolecular interactions and demonstrate the great potential of ionogels for harvesting low-grade heat in human-comfortable humidity environments.
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    High‐Entropy Sulfides as Electrode Materials for Li‐Ion Batteries
    (Weinheim : Wiley-VCH, 2022) Lin, Ling; Wang, Kai; Sarkar, Abhishek; Njel, Christian; Karkera, Guruprakash; Wang, Qingsong; Azmi, Raheleh; Fichtner, Maximilian; Hahn, Horst; Schweidler, Simon; Breitung, Ben
    High-entropy sulfides (HESs) containing 5 equiatomic transition metals (M), with different M:S ratios, are prepared by a facile one-step mechanochemical approach. Two new types of single-phase HESs with pyrite (Pa-3) and orthorhombic (Pnma) structures are obtained and demonstrate a homogeneously mixed solid solution. The straightforward synthesis method can easily tune the desired metal to sulfur ratio for HESs with different stoichiometries, by utilizing the respective metal sulfides, even pure metals, and sulfur as precursor chemicals. The structural details and solid solution nature of HESs are studied by X-ray diffraction, transmission electron microscopy, energy-dispersive X-ray spectroscopy, electron energy loss spectroscopy, X-ray photoelectron spectroscopy, inductively coupled plasma optical emission spectroscopy, and Mössbauer spectroscopy. Since transition metal sulfides are a very versatile material class, here the application of HESs is presented as electrode materials for reversible electrochemical energy storage, in which the HESs show high specific capacities and excellent rate capabilities in secondary Li-ion batteries.
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    In situ detection of cracks during laser powder bed fusion using acoustic emission monitoring
    (Amsterdam : Elsevier, 2022) Seleznev, Mikhail; Gustmann, Tobias; Friebel, Judith Miriam; Peuker, Urs Alexander; Kühn, Uta; Hufenbach, Julia Kristin; Biermann, Horst; Weidner, Anja
    Despite rapid development of laser powder bed fusion (L-PBF) and its monitoring techniques, there is still a lack of in situ crack detection methods, among which acoustic emission (AE) is one of the most sensitive. To elaborate on this topic, in situ AE monitoring was applied to L-PBF manufacturing of a high-strength Al92Mn6Ce2 (at. %) alloy and combined with subsequent X-ray computed tomography. By using a structure borne high-frequency sensor, even a simple threshold-based monitoring was able to detect AE activity associated with cracking, which occurred not only during L-PBF itself, but also after the build job was completed, i.e. in the cooling phase. AE data analysis revealed that crack-related signals can easily be separated from the background noise (e.g. inert gas circulation pump) through their specific shape of a waveform, as well as their energy, skewness and kurtosis. Thus, AE was verified to be a promising method for L-PBF monitoring, enabling to detect formation of cracks regardless of their spatial and temporal occurrence.
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    Beyond Janus Geometry: Characterization of Flow Fields around Nonspherical Photocatalytic Microswimmers
    (Weinheim : Wiley-VCH, 2022) Heckel, Sandra; Bilsing, Clemens; Wittmann, Martin; Gemming, Thomas; Büttner, Lars; Czarske, Jürgen; Simmchen, Juliane
    Catalytic microswimmers that move by a phoretic mechanism in response to a self-induced chemical gradient are often obtained by the design of spherical janus microparticles, which suffer from multi-step fabrication and low yields. Approaches that circumvent laborious multi-step fabrication include the exploitation of the possibility of nonuniform catalytic activity along the surface of irregular particle shapes, local excitation or intrinsic asymmetry. Unfortunately, the effects on the generation of motion remain poorly understood. In this work, single crystalline BiVO4 microswimmers are presented that rely on a strict inherent asymmetry of charge-carrier distribution under illumination. The origin of the asymmetrical flow pattern is elucidated because of the high spatial resolution of measured flow fields around pinned BiVO4 colloids. As a result the flow from oxidative to reductive particle sides is confirmed. Distribution of oxidation and reduction reactions suggests a dominant self-electrophoretic motion mechanism with a source quadrupole as the origin of the induced flows. It is shown that the symmetry of the flow fields is broken by self-shadowing of the particles and synthetic surface defects that impact the photocatalytic activity of the microswimmers. The results demonstrate the complexity of symmetry breaking in nonspherical microswimmers and emphasize the role of self-shadowing for photocatalytic microswimmers. The findings are leading the way toward understanding of propulsion mechanisms of phoretic colloids of various shapes.
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    Regulating Bacterial Behavior within Hydrogels of Tunable Viscoelasticity
    (Weinheim : Wiley-VCH, 2022) Bhusari, Shardul; Sankaran, Shrikrishnan; del Campo, Aránzazu
    Engineered living materials (ELMs) are a new class of materials in which living organism incorporated into diffusive matrices uptake a fundamental role in material's composition and function. Understanding how the spatial confinement in 3D can regulate the behavior of the embedded cells is crucial to design and predict ELM's function, minimize their environmental impact and facilitate their translation into applied materials. This study investigates the growth and metabolic activity of bacteria within an associative hydrogel network (Pluronic-based) with mechanical properties that can be tuned by introducing a variable degree of acrylate crosslinks. Individual bacteria distributed in the hydrogel matrix at low density form functional colonies whose size is controlled by the extent of permanent crosslinks. With increasing stiffness and elastic response to deformation of the matrix, a decrease in colony volumes and an increase in their sphericity are observed. Protein production follows a different pattern with higher production yields occurring in networks with intermediate permanent crosslinking degrees. These results demonstrate that matrix design can be used to control and regulate the composition and function of ELMs containing microorganisms. Interestingly, design parameters for matrices to regulate bacteria behavior show similarities to those elucidated for 3D culture of mammalian cells.
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    Low-cost adaptation options to support green growth in agriculture, water resources, and coastal zones
    ([London] : Macmillan Publishers Limited, part of Springer Nature, 2022) Salack, Seyni; Sanfo, Safiétou; Sidibe, Moussa; Daku, Elidaa K.; Camara, Ibrahima; Dieng, Mame Diarra Bousso; Hien, Koufanou; Torou, Bio Mohamadou; Ogunjobi, Kehinde O.; Sangare, Sheick Ahmed Khalil S. B.; Kouame, Konan Raoul; Koffi, Yao Bernard; Liersch, Stefan; Savadogo, Moumini; Giannini, Alessandra
    The regional climate as it is now and in the future will put pressure on investments in sub-Saharan Africa in water resource management, fisheries, and other crop and livestock production systems. Changes in oceanic characteristics across the Atlantic Ocean will result in remarkable vulnerability of coastal ecology, littorals, and mangroves in the middle of the twenty-first century and beyond. In line with the countries' objectives of creating a green economy that allows reduced greenhouse gas emissions, improved resource efficiency, and prevention of biodiversity loss, we identify the most pressing needs for adaptation and the best adaptation choices that are also clean and affordable. According to empirical data from the field and customized model simulation designs, the cost of these adaptation measures will likely decrease and benefit sustainable green growth in agriculture, water resource management, and coastal ecosystems, as hydroclimatic hazards such as pluviometric and thermal extremes become more common in West Africa. Most of these adaptation options are local and need to be scaled up and operationalized for sustainable development. Governmental sovereign wealth funds, investments from the private sector, and funding from global climate funds can be used to operationalize these adaptation measures. Effective legislation, knowledge transfer, and pertinent collaborations are necessary for their success.
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    Magnetocaloric performance of the three-component Ho1-xErxNi2 (x = 0.25, 0.5, 0.75) Laves phases as composite refrigerants
    ([London] : Macmillan Publishers Limited, part of Springer Nature, 2022) Ćwik, Jacek; Koshkid’ko, Yurii; Nenkov, Konstantin; Tereshina-Chitrova, Evgenia; Małecka, Małgorzata; Weise, Bruno; Kowalska; Karolina
    To date, significant efforts have been put into searching for materials with advanced magnetocaloric properties which show promise as refrigerants and permit realization of efficient cooling. The present study, by an example of Ho1−xErxNi2, develops the concept of magnetocaloric efficiency in the rare-earth Laves-phase compounds. Based on the magneto-thermodynamic properties, their potentiality as components of magnetocaloric composites is illustrated. The determined regularities in the behaviour of the heat capacity, magnetic entropy change, and adiabatic temperature change of the system substantiate reaching high magnetocaloric potentials in a desired temperature range. For the Ho1−xErxNi2 solid solutions, we simulate optimal molar ratios and construct the composites used in magnetic refrigerators performing an Ericsson cycle at low temperatures. The tailored magnetocaloric characteristics are designed and efficient procedures for their manufacturing are developed. Our calculations based on the real empirical data are very promising and open avenue to further experimental studies. Systems showing large magnetocaloric effect (MCE) at low temperatures are of importance due to their potential utilization in refrigeration for gas liquefaction.
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    Effect of Silver Doping on the Superconducting and Structural Properties of YBCO Films Grown by PLD on Different Templates
    (Basel : MDPI, 2022) Shipulin, Ilya A.; Thomas, Aleena Anna; Holleis, Sigrid; Eisterer, Michael; Nielsch, Kornelius; Hühne, Ruben
    We report the local structural and superconducting properties of undoped and Ag-doped YBa2Cu3O6+x (YBCO) films with a thickness of up to 1 µm prepared by pulsed laser deposition on SrTiO3 (STO) single crystals and on ion-beam-assisted deposition (IBAD) and rolling-assisted biaxially textured substrate (RABiTS)-based metal templates. X-ray diffraction demonstrates the high crystalline quality of the films on both single crystalline substrates and metal-based templates, respectively. Although there was only a slight decrease in Tc of up to 1.5 K for the Ag-doped YBCO films on all substrates, we found significant changes in their transport characteristics. The effect of the silver doping mainly depended on the concentration of silver, the type of substrate, and the temperature and magnetic field. In general, the greatest improvement in Jc over a wide range of magnetic fields and temperatures was observed for the 5%Ag-doped YBCO films on STO substrates, showing a significant increase compared to undoped films. Furthermore, a slight Jc improvement was observed for the 2%Ag-doped YBCO films on the RABiTS templates at temperatures below 65 K, whereas Jc decreased for the Ag-doped films on IBAD-MgO-based templates compared to undoped YBCO films. Using detailed electron microscopy studies, small changes in the local microstructure of the Ag-doped YBCO films were revealed; however, no clear correlation was found with the transport properties of the films.
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    Temperature-dependent dynamic compressive properties and failure mechanisms of the additively manufactured CoCrFeMnNi high entropy alloy
    (Oxford : Elsevier Science, 2022) Chen, Hongyu; Liu, Yang; Wang, Yonggang; Li, Zhiguo; Wang, Di; Kosiba, Konrad
    CoCrFeMnNi high entropy alloy (HEA) parts were fabricated by laser powder bed fusion (LPBF), and their dynamic compressive properties at different temperatures as well as the resulting microstructures were analyzed. The HEAs showed an unprecedented strength-ductility combination, especially at a cryogenic temperature of 77 K and a high strain rate of 3000 s−1. Under this testing condition, the yield strength (YS) of the HEAs amounted to 665 MPa. Regardless of the testing temperature, the deformation mechanism of all investigated HEAs was dominated by a synergistic effect consisting of deformation twinning and dislocation pile-up around twins. The fraction of twin boundaries and dislocation density within the deformed microstructure of the HEA correlated with the test temperature. At 77 K, the formation of nanotwins together with dislocation slip prevailed and contributed to pronounced twin-twin and twin-dislocation interactions which effectively restricted the dislocation movement and, hence, contributed to a higher YS as well as strain hardening rate in comparison to that of the HEAs at room temperature of 298 K. The LPBF-fabricated HEAs showed unpronounced thermal softening even at a high testing temperature of 1073 K. Continuous dynamic recrystallization was restricted in the HEA because of its inherent sluggish dislocation kinetics and low stacking fault energy.