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    Current Advances in TiO2-Based Nanostructure Electrodes for High Performance Lithium Ion Batteries
    (Basel : MDPI, 2018-2-6) Madian, Mahmoud; Eychmüller, Alexander; Giebeler, Lars
    The lithium ion battery (LIB) has proven to be a very reliably used system to store electrical energy, for either mobile or stationary applications. Among others, TiO2-based anodes are the most attractive candidates for building safe and durable lithium ion batteries with high energy density. A variety of TiO2 nanostructures has been thoroughly investigated as anodes in LIBs, e.g., nanoparticles, nanorods, nanoneedles, nanowires, and nanotubes discussed either in their pure form or in composites. In this review, we present the recent developments and breakthroughs demonstrated to synthesize safe, high power, and low cost nanostructured titania-based anodes. The reader is provided with an in-depth review of well-oriented TiO2-based nanotubes fabricated by anodic oxidation. Other strategies for modification of TiO2-based anodes with other elements or materials are also highlighted in this report.
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    Structural Aspects of P2-Type Na0.67Mn0.6Ni0.2Li0.2O2 (MNL) Stabilization by Lithium Defects as a Cathode Material for Sodium-Ion Batteries
    (Weinheim : Wiley-VCH, 2021) Yang, Liangtao; Kuo, Liang-Yin; López del Amo, Juan Miguel; Nayak, Prasant Kumar; Mazzio, Katherine A.; Maletti, Sebastian; Mikhailova, Daria; Giebeler, Lars; Kaghazchi, Payam; Rojo, Teófilo; Adelhelm, Philipp
    A known strategy for improving the properties of layered oxide electrodes in sodium-ion batteries is the partial substitution of transition metals by Li. Herein, the role of Li as a defect and its impact on sodium storage in P2-Na0.67Mn0.6Ni0.2Li0.2O2 is discussed. In tandem with electrochemical studies, the electronic and atomic structure are studied using solid-state NMR, operando XRD, and density functional theory (DFT). For the as-synthesized material, Li is located in comparable amounts within the sodium and the transition metal oxide (TMO) layers. Desodiation leads to a redistribution of Li ions within the crystal lattice. During charging, Li ions from the Na layer first migrate to the TMO layer before reversing their course at low Na contents. There is little change in the lattice parameters during charging/discharging, indicating stabilization of the P2 structure. This leads to a solid-solution type storage mechanism (sloping voltage profile) and hence excellent cycle life with a capacity of 110 mAh g-1 after 100 cycles. In contrast, the Li-free compositions Na0.67Mn0.6Ni0.4O2 and Na0.67Mn0.8Ni0.2O2 show phase transitions and a stair-case voltage profile. The capacity is found to originate from mainly Ni3+/Ni4+ and O2-/O2-δ redox processes by DFT, although a small contribution from Mn4+/Mn5+ to the capacity cannot be excluded. © 2021 The Authors. Advanced Functional Materials published by Wiley-VCH GmbH
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    Progress and challenges in using sustainable carbon anodes in rechargeable metal-ion batteries
    (Amsterdam [u.a.] : Elsevier, 2021) Soltani, Niloofar; Bahrami, Amin; Giebeler, Lars; Gemming, Thomas; Mikhailova, Daria
    Rechargeable lithium-ion batteries (LIBs) are one of the most promising alternatives to effectively bypass fossil fuels. However, long-term energy application of LIBs could be restricted in the future due to the increased production cost of LIB arising from the shortage and inaccessibility of Li in the Earth's crust. Na or K have been considered as substitutes for Li but in spite of their natural abundance, they suffer from low gravimetric/volumetric energy density. An alternative to increase the efficiency of sodium-ion battery (SIBs) and potassium-ion battery (KIBs) is to focus on finding the high‐performing negative electrode, the anode. The large volume changes of alloying and conversion type anodes for KIBs and SIBs make hard carbons to a better option on this regard than usual graphitic carbons, but a key obstacle is the reliance on unsustainable sources. Thus, biomass-derived carbon could offer a promising alternative, and it has indeed been in the focus of much recent work. This review highlights the recent advances in using carbon extracted from various biomass sources in rechargeable Li-, Na-, and K-ion batteries. Maximizing the energy and power densities as well as the lifetime of carbon anodes require an exploration of the right balance between carbon structures, pore morphology, chemical composition and alkali metal-ion storage. Thus, in this review, first, we take stock of key challenges and opportunities to extract carbon from various plants structural components and identify the extracted carbon structure compared to graphite-like structure. Then, we provide an overview on morphological and structural modification of the extracted carbons. Finally, we show how the physicochemical properties, structural alignment and morphological variation of the biomass-derived carbon can affect the storage mechanism and electrochemical performance. The extensive overview of this topic provided here is expected to stimulate further work on environmentally friendly battery design and towards the optimization of the battery performance. Electrode materials in alkali-metal-ion batteries that are based on biomass-derived carbon may allow not only a technical breakthrough, but also an ethically and socially acceptable product.
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    High-Pressure-Sintering-Induced Microstructural Engineering for an Ultimate Phonon Scattering of Thermoelectric Half-Heusler Compounds
    (Weinheim : Wiley-VCH, 2021) He, Ran; Zhu, Taishan; Ying, Pingjun; Chen, Jie; Giebeler, Lars; Kühn, Uta; Grossman, Jeffrey C.; Wang, Yumei; Nielsch, Kornelius
    Thermal management is of vital importance in various modern technologies such as portable electronics, photovoltaics, and thermoelectric devices. Impeding phonon transport remains one of the most challenging tasks for improving the thermoelectric performance of certain materials such as half-Heusler compounds. Herein, a significant reduction of lattice thermal conductivity (κL) is achieved by applying a pressure of ≈1 GPa to sinter a broad range of half-Heusler compounds. Contrasting with the common sintering pressure of less than 100 MPa, the gigapascal-level pressure enables densification at a lower temperature, thus greatly modifying the structural characteristics for an intensified phonon scattering. A maximum κL reduction of ≈83% is realized for HfCoSb from 14 to 2.5 W m−1 K−1 at 300 K with more than 95% relative density. The realized low κL originates from a remarkable grain-size refinement to below 100 nm together with the abundant in-grain defects, as determined by microscopy investigations. This work uncovers the phonon transport properties of half-Heusler compounds under unconventional microstructures, thus showing the potential of high-pressure compaction in advancing the performance of thermoelectric materials.