03 Fakultät Chemie

Permanent URI for this collectionhttps://elib.uni-stuttgart.de/handle/11682/4

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Subject: search.filters.subject.660Institute: search.filters.UBSInstitut.Max-Planck-Institut für Festkörperforschung

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    Binder-free V2O5 cathode for high energy density rechargeable aluminum-ion batteries
    (2020) Diem, Achim M.; Fenk, Bernhard; Bill, Joachim; Burghard, Zaklina
    Nowadays, research on electrochemical storage systems moves into the direction of post-lithium-ion batteries, such as aluminum-ion batteries, and the exploration of suitable materials for such batteries. Vanadium pentoxide (V2O5) is one of the most promising host materials for the intercalation of multivalent ions. Here, we report on the fabrication of a binder-free and self-supporting V2O5 micrometer-thick paper-like electrode material and its use as the cathode for rechargeable aluminum-ion batteries. The electrical conductivity of the cathode was significantly improved by a novel in-situ and self-limiting copper migration approach into the V2O5 structure. This process takes advantage of the dissolution of Cu by the ionic liquid-based electrolyte, as well as the presence of two different accommodation sites in the nanostructured V2O5 available for aluminum-ions and the migrated Cu. Furthermore, the advanced nanostructured cathode delivered a specific discharge capacity of up to ~170 mAh g-1 and the reversible intercalation of Al3+ for more than 500 cycles with a high Coulomb efficiency reaching nearly 100%. The binder-free concept results in an energy density of 74 Wh kg-1, which shows improved energy density in comparison to the so far published V2O5-based cathodes. Our results provide valuable insights for the future design and development of novel binder-free and self-supporting electrodes for rechargeable multivalent metal-ion batteries associating a high energy density, cycling stability, safety and low cost.
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    Asymmetric Rh diene catalysis under confinement : isoxazole ring‐contraction in mesoporous solids
    (2024) Marshall, Max; Dilruba, Zarfishan; Beurer, Ann‐Katrin; Bieck, Kira; Emmerling, Sebastian; Markus, Felix; Vogler, Charlotte; Ziegler, Felix; Fuhrer, Marina; Liu, Sherri S. Y.; Kousik, Shravan R.; Frey, Wolfgang; Traa, Yvonne; Bruckner, Johanna R.; Plietker, Bernd; Buchmeiser, Michael R.; Ludwigs, Sabine; Naumann, Stefan; Atanasova, Petia; Lotsch, Bettina V.; Zens, Anna; Laschat, Sabine
    Covalent immobilization of chiral dienes in mesoporous solids for asymmetric heterogeneous catalysis is highly attractive. In order to study confinement effects in bimolecular vs monomolecular reactions, a series of pseudo‐C2‐symmetrical tetrahydropentalenes was synthesized and immobilized via click reaction on different mesoporous solids (silica, carbon, covalent organic frameworks) and compared with homogeneous conditions. Two types of Rh‐catalyzed reactions were studied: (a) bimolecular nucleophilic 1,2‐additions of phenylboroxine to N‐tosylimine and (b) monomolecular isomerization of isoxazole to 2H‐azirne. Polar support materials performed better than non‐polar ones. Under confinement, bimolecular reactions showed decreased yields, whereas yields in monomolecular reactions were only little affected. Regarding enantioselectivity the opposite trend was observed, i. e. effective enantiocontrol for bimolecular reactions but only little control for monomolecular reactions was found.
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    Realization of a classical Ruddlesden Popper type bilayer nickelate in Sr3Ni2-xAlxO7-δ with unusual Ni4+
    (2024) Yilmaz, Hasan; Küster, Kathrin; Starke, Ulrich; Clemens, Oliver; Isobe, Masahiko; Puphal, Pascal
    The discovery of 80 K superconductivity in bilayer La3Ni2O7 at pressures greater than 14 GPa presents a unique opportunity to study a novel class of high-temperature superconductors. Therefore, other bilayer nickelates following the classical (T4+) Ruddlesden-Popper (RP) series of Sr3Ni2O7 would present an interesting new candidate. In this work, we study the stabilization of RP n = 2 phase in Sr3Ni2-xAlxO7-δ, via floating zone growth of crystals. With powder and single-crystal XRD, we study the stability range of the RP-type phase. Our Thermogravimetric Analysis (TGA), X-ray photoelectron spectroscopy (XPS) and gas extraction studies reveal a remarkably high oxidation state of Ni4+ stabilized by chemical strain from Al. The obtained black crystals are insulating in transport and show a magnetic transition around 12 K.
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    Towards recycling of all‐solid‐state batteries with argyrodite sulfide electrolytes : insights into electrolyte and electrode degradation in dissolution‐based separation processes
    (2025) Wissel, Kerstin; Hu, Zian; Wu, Xuebin; Jacob, Martine; Küster, Kathrin; Starke, Ulrich; Clemens, Oliver
    All‐solid‐state Li‐ion batteries (ASSBs) represent a promising leap forward in battery technology, rapidly advancing in development. Among the various solid electrolytes, argyrodite thiophosphates Li6PS5X (X=Cl, Br, I) stand out due to their high ionic conductivity, structural flexibility, and compatibility with a range of electrode materials, making them ideal candidates for efficient and scalable battery applications. However, despite significant performance advancements, the sustainability and recycling of ASSBs remain underexplored, posing a critical challenge for achieving efficient circular processes. This study investigates the dissolution‐based separation and recovery of argyrodite thiophosphate electrolytes and transition metal oxide electrode materials as a potential recycling strategy for ASSBs. A focus is set on the impact of solvent treatments on the recrystallization behavior of these electrolytes. Furthermore, the interactions between dissolved argyrodite thiophosphates and various transition metal oxide electrode materials (LiCoO2, LiMn2O4, LiNi0.8Mn0.1Co0.1O2, LiFePO4 and Li4Ti5O12) is examined to assess their influence on the functional properties of both the electrolytes and electrode materials. Structural, compositional and morphological changes are analyzed using X‐ray diffraction, scanning electron microscopy, energy‐dispersive X‐ray spectroscopy, inductively coupled plasma mass spectrometry and X‐ray photoelectron spectroscopy. Our findings provide insights into the complexities of recycling ASSBs, but also highlight the potential for developing efficient, sustainable recycling processes.