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- ItemThe Role of Al2O3 ALD Coating on Sn-Based Intermetallic Anodes for Rate Capability and Long-Term Cycling in Lithium-Ion Batteries(Weinheim : Wiley-VCH, 2022) Soltani, Niloofar; Abbas, Syed Muhammad; Hantusch, Martin; Lehmann, Sebastian; Nielsch, Kornelius; Bahrami, Amin; Mikhailova, DariaThe electrochemical performances of CoSn2 and Ni3Sn4 as potential anode materials in lithium-ion batteries (LIBs) are investigated using varying thicknesses of an alumina layer deposited by the atomic layer deposition (ALD) technique. Rate capability results showed that at high current densities, Al2O3-coated CoSn2 and Ni3Sn4 electrodes after 10-ALD cycles outperformed uncoated materials. The charge capacities of coated CoSn2 and Ni3Sn4 electrodes are 571 and 134 mAh g−1, respectively, at a high current density of 5 A g−1, while the capacities of uncoated electrodes are 363 and 11 mAh g−1. When the current density is reduced to 1 A g−1, however, the cycling performances of Al2O3-coated CoSn2 and Ni3Sn4 electrodes fade faster after almost 40 cycles than uncoated electrodes. The explanation is found in the composition of the solid-electrolyte interface (SEI), which strongly depends on the current rate. Thus, X-ray photoelectron spectroscopy analysis of SEI layers on coated samples cycles at a low current density of 0.1 Ag−1, revealed organic carbonates as major products, which probably have a low ionic conductivity. In contrast, the SEI of coated materials cycled at 5 Ag−1 consists mostly of mixed inorganic/organic fluorine-rich Al-F and C-F species facilitating a higher ionic transport, which improves electrochemical performance.
- ItemSelf‐Patterning of Multifunctional Heusler Membranes by Dewetting(Weinheim : Wiley-VCH, 2021) Lünser, Klara; Diestel, Anett; Nielsch, Kornelius; Fähler, SebastianNi-Mn-based Heusler alloys are an emerging class of materials which enable actuation by (magnetic) shape memory effects, magnetocaloric cooling, and thermomagnetic energy harvesting. Multifunctional materials have a particular advantage for miniaturization since their functionality is already built within the material. However, often complex microtechnological processing is required to bring these materials into shape. Here, self-organized formation of single crystalline membranes having arrays of rectangular holes with high aspect ratio is demonstrated. Dewetting avoids the need for complicated processing and allows to prepare freestanding Ni–Mn–Ga–Co membranes. These membranes are martensitic and magnetic, and their functional properties are not disturbed by self-patterning. Feature sizes of these membranes can be tailored by film thickness and heat treatment, and the tendencies can be explained with dewetting. As an outlook, the advantages of these multifunctional membranes for magnetocaloric and thermomagnetic microsystems are sketched. © 2021 The Authors. Advanced Materials Interfaces published by Wiley-VCH GmbH
- ItemBuilding Hierarchical Martensite(Weinheim : Wiley-VCH, 2020) Schwabe, Stefan; Niemann, Robert; Backen, Anja; Wolf, Daniel; Damm, Christine; Walter, Tina; Seiner, Hanuš; Heczko, Oleg; Nielsch, Kornelius; Fähler, SebastianMartensitic materials show a complex, hierarchical microstructure containing structural domains separated by various types of twin boundaries. Several concepts exist to describe this microstructure on each length scale, however, there is no comprehensive approach bridging the whole range from the nano- up to the macroscopic scale. Here, it is described for a Ni-Mn-based Heusler alloy how this hierarchical microstructure is built from scratch with just one key parameter: the tetragonal distortion of the basic building block at the atomic level. Based on this initial block, five successive levels of nested building blocks are introduced. At each level, a larger building block is formed by twinning the preceding one to minimize the relevant energy contributions locally. This naturally explains the coexistence of different types of twin boundaries. The scale-bridging approach of nested building blocks is compared with experiments in real and reciprocal space. The approach of nested building blocks is versatile as it can be applied to the broad class of functional materials exhibiting diffusionless transformations. © 2020 The Authors. Advanced Functional Materials published by Wiley-VCH GmbH
- ItemTransparent Power-Generating Windows Based on Solar-Thermal-Electric Conversion(Weinheim : Wiley-VCH, 2021) Zhang, Qihao; Huang, Aibin; Ai, Xin; Liao, Jincheng; Song, Qingfeng; Reith, Heiko; Cao, Xun; Fang, Yueping; Schierning, Gabi; Nielsch, Kornelius; Bai, Shengqiang; Chen, LidongIntegrating transparent solar-harvesting systems into windows can provide renewable on-site energy supply without altering building aesthetics or imposing further design constraints. Transparent photovoltaics have shown great potential, but the increased transparency comes at the expense of reduced power-conversion efficiency. Here, a new technology that overcomes this limitation by combining solar-thermal-electric conversion with a material's wavelength-selective absorption is presented. A wavelength-selective film consisting of Cs0.33WO3 and resin facilitates high visible-light transmittance (up to 88%) and outstanding ultraviolet and infrared absorbance, thereby converting absorbed light into heat without sacrificing transparency. A prototype that couples the film with thermoelectric power generation produces an extraordinary output voltage of ≈4 V within an area of 0.01 m2 exposed to sunshine. Further optimization design and experimental verification demonstrate high conversion efficiency comparable to state-of-the-art transparent photovoltaics, enriching the library of on-site energy-saving and transparent power generation.
- ItemCurrent State-of-the-Art in the Interface/Surface Modification of Thermoelectric Materials(Weinheim : Wiley-VCH, 2021) He, Shiyang; Lehmann, Sebastian; Bahrami, Amin; Nielsch, KorneliusThermoelectric (TE) materials are prominent candidates for energy converting applications due to their excellent performance and reliability. Extensive efforts for improving their efficiency in single-/multi-phase composites comprising nano/micro-scale second phases are being made. The artificial decoration of second phases into the thermoelectric matrix in multi-phase composites, which is distinguished from the second-phase precipitation occurring during the thermally equilibrated synthesis of TE materials, can effectively enhance their performance. Theoretically, the interfacial manipulation of phase boundaries can be extended to a wide range of materials. High interface densities decrease thermal conductivity when nano/micro-scale grain boundaries are obtained and certain electronic structure modifications may increase the power factor of TE materials. Based on the distribution of second phases on the interface boundaries, the strategies can be divided into discontinuous and continuous interfacial modifications. The discontinuous interfacial modifications section in this review discusses five parts chosen according to their dispersion forms, including metals, oxides, semiconductors, carbonic compounds, and MXenes. Alternatively, gas- and solution-phase process techniques are adopted for realizing continuous surface changes, like the core–shell structure. This review offers a detailed analysis of the current state-of-the-art in the field, while identifying possibilities and obstacles for improving the performance of TE materials.
- ItemControl of Positive and Negative Magnetoresistance in Iron Oxide : Iron Nanocomposite Thin Films for Tunable Magnetoelectric Nanodevices(2020) Nichterwitz, Martin; Honnali, Shashank; Zehner, Jonas; Schneider, Sebastian; Pohl, Darius; Schiemenz, Sandra; Goennenwein, Sebastian T.B.; Nielsch, Kornelius; Leistner, KarinThe perspective of energy-efficient and tunable functional magnetic nanostructures has triggered research efforts in the fields of voltage control of magnetism and spintronics. We investigate the magnetotransport properties of nanocomposite iron oxide/iron thin films with a nominal iron thickness of 5-50 nm and find a positive magnetoresistance at small thicknesses. The highest magnetoresistance was found for 30 nm Fe with +1.1% at 3 T. This anomalous behavior is attributed to the presence of Fe3O4-Fe nanocomposite regions due to grain boundary oxidation. At the Fe3O4/Fe interfaces, spin-polarized electrons in the magnetite can be scattered and reoriented. A crossover to negative magnetoresistance (-0.11%) is achieved at a larger thickness (>40 nm) when interface scattering effects become negligible as more current flows through the iron layer. Electrolytic gating of this system induces voltage-triggered redox reactions in the Fe3O4 regions and thereby enables voltage-tuning of the magnetoresistance with the locally oxidized regions as the active tuning elements. In the low-magnetic-field region (<1 T), a crossover from positive to negative magnetoresistance is achieved by a voltage change of only 1.72 V. At 3 T, a relative change of magnetoresistance about -45% during reduction was achieved for the 30 nm Fe sample. The present low-voltage approach signifies a step forward to practical and tunable room-temperature magnetoresistance-based nanodevices, which can boost the development of nanoscale and energy-efficient magnetic field sensors with high sensitivity, magnetic memories, and magnetoelectric devices in general. Copyright © 2020 American Chemical Society.
- ItemStructural and Electric Properties of Epitaxial Na0.5Bi0.5TiO3-Based Thin Films(Basel : MDPI, 2021) Magalhaes, Bruno; Engelhardt, Stefan; Molin, Christian; Gebhardt, Sylvia E.; Nielsch, Kornelius; Hühne, RubenSubstantial efforts are dedicated worldwide to use lead-free materials for environmentally friendly processes in electrocaloric cooling. Whereas investigations on bulk materials showed that Na0.5Bi0.5TiO3 (NBT)-based compounds might be suitable for such applications, our aim is to clarify the feasibility of epitaxial NBT-based thin films for more detailed investigations on the correlation between the composition, microstructure, and functional properties. Therefore, NBT-based thin films were grown by pulsed laser deposition on different single crystalline substrates using a thin epitaxial La0.5Sr0.5CoO3 layer as the bottom electrode for subsequent electric measurements. Structural characterization revealed an undisturbed epitaxial growth of NBT on lattice-matching substrates with a columnar microstructure, but high roughness and increasing grain size with larger film thickness. Dielectric measurements indicate a shift of the phase transition to lower temperatures compared to bulk samples as well as a reduced permittivity and increased losses at higher temperatures. Whereas polarization loops taken at −100 °C revealed a distinct ferroelectric behavior, room temperature data showed a significant resistive contribution in these measurements. Leakage current studies confirmed a non-negligible conductivity between the electrodes, thus preventing an indirect characterization of the electrocaloric properties of these films.
- ItemInfluence of Nanoparticle Processing on the Thermoelectric Properties of (BixSb1−X)2Te3 Ternary Alloys(Weinheim : Wiley-VCH, 2021) Salloum, Sarah; Bendt, Georg; Heidelmann, Markus; Loza, Kateryna; Bayesteh, Samaneh; Izadi, M. Sepideh; Patrick, Kawulok; He, Ran; Schlörb, Heike; Perez, Nicolas; Reith, Heiko; Nielsch, Kornelius; Schierning, Gabi; Schulz, StephanThe synthesis of phase‐pure ternary solutions of tetradymite‐type materials (BixSb1−x)2Te3 (x=0.25; 0.50; 0.75) in an ionic liquid approach has been carried out. The nanoparticles are characterized by means of energy‐dispersive X‐ray spectroscopy (EDX), powder X‐ray diffraction (PXRD), scanning electron microscopy (SEM), and transmission electron microscopy. In addition, the role of different processing approaches on the thermoelectric properties ‐ Seebeck coefficient as well as electrical and thermal conductivity ‐ is demonstrated.
- ItemCore–Shell Structures Prepared by Atomic Layer Deposition on GaAs Nanowires(Basel : MDPI, 2022) Ursaki, Veaceslav V.; Lehmann, Sebastian; Zalamai, Victor V.; Morari, Vadim; Nielsch, Kornelius; Tiginyanu, Ion M.; Monaico, Eduard V.GaAs nanowire arrays have been prepared by anodization of GaAs substrates. The nanowires produced on (111)B GaAs substrates were found to be oriented predominantly perpendicular to the substrate surface. The prepared nanowire arrays have been coated with thin ZnO or TiO2 layers by means of thermal atomic layer deposition (ALD), thus coaxial core–shell hybrid structures are being fabricated. The hybrid structures have been characterized by scanning electron microscopy (SEM) for the morphology investigations, by Energy Dispersive X-ray (EDX) and X-ray diffraction (XRD) analysis for the composition and crystal structure assessment, and by photoluminescence (PL) spectroscopy for obtaining an insight on emission polarization related to different recombination channels in the prepared core–shell structures.
- ItemAero-TiO2 Prepared on the Basis of Networks of ZnO Tetrapods(Basel : MDPI, 2022) Ciobanu, Vladimir; Ursaki, Veaceslav V.; Lehmann, Sebastian; Braniste, Tudor; Raevschi, Simion; Zalamai, Victor V.; Monaico, Eduard V.; Colpo, Pascal; Nielsch, Kornelius; Tiginyanu, Ion M.In this paper, new aeromaterials are proposed on the basis of titania thin films deposited using atomic layer deposition (ALD) on a sacrificial network of ZnO microtetrapods. The technology consists of two technological steps applied after ALD, namely, thermal treatment at different temperatures and etching of the sacrificial template. Two procedures are applied for etching, one of which is wet etching in a citric acid aqua solution, while the other one is etching in a hydride vapor phase epitaxy (HVPE) system with HCl and hydrogen chemicals. The morphology, composition, and crystal structure of the produced aeromaterials are investigated depending on the temperature of annealing and the sequence of the technological steps. The performed photoluminescence analysis suggests that the developed aeromaterials are potential candidates for photocatalytic applications.