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We present the successful synthesis and characterization of a one-dimensional high-entropy oxide (1D-HEO) exhibiting nanoribbon morphology. These 1D-HEO nanoribbons exhibit high structural stability at elevated temperatures (to 1000°C), elevated pressures (to 12 gigapascals), and long exposure to harsh acid or base chemical environments. Moreover, they exhibit notable mechanical properties, with an excellent modulus of resilience reaching 40 megajoules per cubic meter. High-pressure experiments reveal an intriguing transformation of the 1D-HEO nanoribbons from orthorhombic to cubic structures at 15 gigapascals followed by the formation of fully amorphous HEOs above 30 gigapascals, which are recoverable to ambient conditions. These transformations introduce additional entropy (structural disorder) besides configurational entropy. This finding offers a way to create low-dimensional, resilient, and high-entropy materials. 

Abstract Li‐rich disordered rocksalt (DRS) oxyfluorides have emerged as promising high‐energy cathode materials for lithium‐ion batteries. While a high level of fluorination in DRS materials offers performance advantages, it can only be achieved via mechanochemical synthesis, which poses challenges of reproducibility and scalability. The definition of relationships between fluorination and structural stability is required to devise alternative methods that overcome these challenges. In this study, the thermal evolution of three highly fluorinated phases, Li₂TMO₂F (TM = Mn, Co, and Ni), is investigated in an inert atmosphere. Diffraction and spectroscopic techniques are utilized to examine their electronic and chemical states up until conditions of decomposition. The analysis reveals that the materials phase‐separate above 400 °C, at most. It is also observed that heat‐treated DRS materials exhibit intricate changes in the local coordination of the metals, including their spin, and ordering compared to the pristine states. The changes upon annealing are accompanied by a modulation of the voltage profile, including reduced hysteresis, when used as electrodes. These results provide an in‐depth understanding of the fundamental crystal chemistry of DRS oxyfluorides in view of their promising role as the next generation of Li‐ion cathodes. 

Abstract Lithium‐rich transition metal chalcogenides are witnessing a revival as candidates for Li‐ion cathode materials, spurred by the boost in their capacities from transcending conventional redox processes based on cationic states and tapping into additional chalcogenide states. A particularly striking case is Li₂TiS_3‐ySe_y, which features a d⁰metal. While the end members are expectedly inactive, substantial capacities are measured when both Se and S are present. Using X‐ray absorption spectroscopy, it is shown that the electronic structure of Li₂TiS_3‐ySe_yis not a simple combination of the end members. The data confirm previous hypotheses that, in Li₂TiS_2.4Se_0.6, this behavior is underpinned by concurrent and reversible redox of only S and Se, and identify key electronic states. Moreover, wavelet transforms of the extended X‐ray absorption fine structure provide direct evidence of the formation of short Se–Se units upon charging. The study uncovers the underpinnings of this intriguing reactivity and highlights the richness of redox chemistry in complex solids.