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The Role of Al2O3 ALD Coating on Sn-Based Intermetallic Anodes for Rate Capability and Long-Term Cycling in Lithium-Ion Batteries

2022, Soltani, Niloofar, Abbas, Syed Muhammad, Hantusch, Martin, Lehmann, Sebastian, Nielsch, Kornelius, Bahrami, Amin, Mikhailova, Daria

The 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.

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Current State-of-the-Art in the Interface/Surface Modification of Thermoelectric Materials

2021, He, Shiyang, Lehmann, Sebastian, Bahrami, Amin, Nielsch, Kornelius

Thermoelectric (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.

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Magnetic Properties of GaAs/NiFe Coaxial Core-Shell Structures

2022, Monaico, Eduard V., Morari, Vadim, Kutuzau, Maksim, Ursaki, Veaceslav V., Nielsch, Kornelius, Tiginyanu, Ion M.

Uniform nanogranular NiFe layers with Ni contents of 65%, 80%, and 100% have been electroplated in the potentiostatic deposition mode on both planar substrates and arrays of nanowires prepared by the anodization of GaAs substrates. The fabricated planar and coaxial core-shell ferromagnetic structures have been investigated by means of scanning electron microscopy (SEM) and vibrating sample magnetometry (VSM). To determine the perspectives for applications, a comparative analysis of magnetic properties, in terms of the saturation and remanence moment, the squareness ratio, and the coercivity, was performed for structures with different Ni contents.

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On Curie temperature of B20-MnSi films

2022, Li, Zichao, Yuan, Ye, Begeza, Viktor, Rebohle, Lars, Helm, Manfred, Nielsch, Kornelius, Prucnal, Slawomir, Zhou, Shengqiang

B20-type MnSi is the prototype magnetic skyrmion material. Thin films of MnSi show a higher Curie temperature than their bulk counterpart. However, it is not yet clear what mechanism leads to the increase of the Curie temperature. In this work, we grow MnSi films on Si(100) and Si(111) substrates with a broad variation in their structures. By controlling the Mn thickness and annealing parameters, the pure MnSi phase of polycrystalline and textured nature as well as the mixed phase of MnSi and MnSi1.7 are obtained. Surprisingly, all these MnSi films show an increased Curie temperature of up to around 43 K. The Curie temperature is likely independent of the structural parameters within our accessibility including the film thickness above a threshold, strain, cell volume and the mixture with MnSi1.7. However, a pronounced phonon softening is observed for all samples, which can tentatively be attributed to slight Mn excess from stoichiometry, leading to the increased Curie temperature.

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Self‐Patterning of Multifunctional Heusler Membranes by Dewetting

2021, Lünser, Klara, Diestel, Anett, Nielsch, Kornelius, Fähler, Sebastian

Ni-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

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Effect of Silver Doping on the Superconducting and Structural Properties of YBCO Films Grown by PLD on Different Templates

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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Efficient and affordable thermomagnetic materials for harvesting low grade waste heat

2021, Dzekan, Daniel, Waske, Anja, Nielsch, Kornelius, Fähler, Sebastian

Industrial processes release substantial quantities of waste heat, which can be harvested to generate electricity. At present, the conversion of low grade waste heat to electricity relies solely on thermoelectric materials, but such materials are expensive and have low thermodynamic efficiencies. Although thermomagnetic materials may offer a promising alternative, their performance remains to be evaluated, thereby hindering their real-world application. Here, the efficiency and cost effectiveness of thermomagnetic materials are evaluated for the usage in motors, oscillators, and generators for converting waste heat to electricity. The analysis reveals that up to temperature differences of several 10 K, the best thermomagnetic materials have the potential to compete with thermoelectric materials. Importantly, it is found that the price per watt of some thermomagnetic materials is much lower compared to that of present-day thermoelectrics, which can become competitive with conventional power plants. This materials library enables the selection of the best available thermomagnetic materials for harvesting waste heat and gives guidelines for their future development.

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Transparent Power-Generating Windows Based on Solar-Thermal-Electric Conversion

2021, Zhang, Qihao, Huang, Aibin, Ai, Xin, Liao, Jincheng, Song, Qingfeng, Reith, Heiko, Cao, Xun, Fang, Yueping, Schierning, Gabi, Nielsch, Kornelius, Bai, Shengqiang, Chen, Lidong

Integrating 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.

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Europium Clustering and Glassy Magnetic Behavior in Inorganic Clathrate-VIII Eu8Ga16Ge30

2022, Pérez, Nicolás, Sahoo, Manaswini, Schierning, Gabi, Nielsch, Kornelius, Nolas, George S.

The temperature- and field-dependent, electrical and thermal properties of inorganic clathrate-VIII Eu8Ga16Ge30 were investigated. The type VIII clathrates were obtained from the melt of elements as reported previously. Specifically, the electrical resistivity data show hysteretic magnetoresistance at low temperatures, and the Seebeck coefficient and Hall data indicate magnetic interactions that affect the electronic structure in this material. Heat capacity and thermal conductivity data corroborate these findings and reveal the complex behavior due to Eu2+ magnetic ordering and clustering from approximately 13 to 4 K. Moreover, the low-frequency dynamic response indicates Eu8Ga16Ge30 to be a glassy magnetic system. In addition to advancing our fundamental understanding of the physical properties of this material, our results can be used to further the research for potential applications of interest in the fields of magnetocalorics or thermoelectrics.

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Waste Recycling in Thermoelectric Materials

2020, Bahrami, Amin, Schierning, Gabi, Nielsch, Kornelius

Thermoelectric (TE) technology enables the efficient conversion of waste heat generated in homes, transport, and industry into promptly accessible electrical energy. Such technology is thus finding increasing applications given the focus on alternative sources of energy. However, the synthesis of TE materials relies on costly and scarce elements, which are also environmentally damaging to extract. Moreover, spent TE modules lead to a waste of resources and cause severe pollution. To address these issues, many laboratory studies have explored the synthesis of TE materials using wastes and the recovery of scarce elements from spent modules, e.g., utilization of Si slurry as starting materials, development of biodegradable TE papers, and bacterial recovery and recycling of tellurium from spent TE modules. Yet, the outcomes of such work have not triggered sustainable industrial practices to the extent needed. This paper provides a systematic overview of the state of the art with a view to uncovering the opportunities and challenges for expanded application. Based on this overview, it explores a framework for synthesizing TE materials from waste sources with efficiencies comparable to those made from raw materials.