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  1. Abstract

    Understanding the behavior of lithium‐ion batteries (LIBs) under extreme conditions, for example, low temperature, is key to broad adoption of LIBs in various application scenarios. LIBs, poor performance at low temperatures is often attributed to the inferior lithium‐ion transport in the electrolyte, which has motivated new electrolyte development as well as the battery preheating approach that is popular in electric vehicles. A significant irrevocable capacity loss, however, is not resolved by these measures nor well understood. Herein, multiphase, multiscale chemomechanical behaviors in composite LiNixMnyCozO2(NMC,x +y +z = 1) cathodes at extremely low temperatures are systematically elucidated. The low‐temperature storage of LIBs can result in irreversible structural damage in active electrodes, which can negatively impact the subsequent battery cycling performance at ambient temperature. Beside developing electrolytes that have stable performance, designing batteries for use in a wide temperature range also calls for the development of electrode components that are structurally and morphologically robust when the cell is switched between different temperatures.

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  2. Abstract

    Benefiting from abundant resource reserves and considerable theoretical capacity, sodium (Na) metal is a strong anode candidate for low‐cost, large‐scale energy storage applications. However, extensive volume change and mossy/dendritic growth during Na electrodeposition have impeded the practical application of Na metal batteries. Herein, a self‐sodiophilic carbon host, lignin‐derived carbon nanofiber (LCNF), is reported to accommodate Na metal through an infiltration method. Na metal is completely encapsulated in the 3D space of the LCNF host, where the strong interaction between LCNF and Na metal is mediated by the self‐sodiophilic sites. The resulting LCNF@Na electrode delivers good cycling stability with a low voltage hysteresis and a dendrite‐free morphology in commercial carbonate‐based electrolytes. When interfaced with O3‐NaNi0.33Mn0.33Fe0.33O2and P2‐Na0.7Ni0.33Mn0.55Fe0.1Ti0.02O2cathodes in full cell Na metal batteries, the LCNF@Na electrode enables high capacity retentions, long cycle life, and good rate capability. Even in a “lean” Na anode environment, the full cells can still deliver good electrochemical performance. The overall stable battery performance, based on a self‐sodiophilic, biomass‐derived carbon host, illuminates a promising path towards enabling low‐cost Na metal batteries.

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  3. Abstract

    Manganese‐rich layered oxide materials hold great potential as low‐cost and high‐capacity cathodes for Na‐ion batteries. However, they usually form a P2 phase and suffer from fast capacity fade. In this work, an O3 phase sodium cathode has been developed out of a Li and Mn‐rich layered material by leveraging the creation of transition metal (TM) and oxygen vacancies and the electrochemical exchange of Na and Li. The Mn‐rich layered cathode material remains primarily O3 phase during sodiation/desodiation and can have a full sodiation capacity of ca. 220 mAh g−1. It delivers ca. 160 mAh g−1specific capacity between 2–3.8 V with >86 % retention over 250 cycles. The TM and oxygen vacancies pre‐formed in the sodiated material enables a reversible migration of TMs from the TM layer to the tetrahedral sites in the Na layer upon de‐sodiation and sodiation. The migration creates metastable states, leading to increased kinetic barrier that prohibits a complete O3‐P3 phase transition.

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  4. Abstract

    Crystallographic defects exist in many redox active energy materials, e.g., battery and catalyst materials, which significantly alter their chemical properties for energy storage and conversion. However, there is lack of quantitative understanding of the interrelationship between crystallographic defects and redox reactions. Herein, crystallographic defects, such as geometrically necessary dislocations, are reported to influence the redox reactions in battery particles through single‐particle, multimodal, and in situ synchrotron measurements. Through Laue X‐ray microdiffraction, many crystallographic defects are spatially identified and statistically quantified from a large quantity of diffraction patterns in many layered oxide particles, including geometrically necessary dislocations, tilt boundaries, and mixed defects. The in situ and ex situ measurements, combining microdiffraction and X‐ray spectroscopy imaging, reveal that LiCoO2particles with a higher concentration of geometrically necessary dislocations provide deeper charging reactions, indicating that dislocations may facilitate redox reactions in layered oxides during initial charging. The present study illustrates that a precise control of crystallographic defects and their distribution can potentially promote and homogenize redox reactions in battery materials.

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  5. Cushing, Scott (Ed.)

    This feature page is intended to let ECS award winning students and post-docs write a primary-author perspective on their field, their work, and where they believe things are going. This month we highlight the work of Muhammad Mominur Rahman, the Battery Division 2021 Student Research Award winner.

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  6. The diffusion layer created by transition metal (TM) dissolution is ubiquitous at the electrochemical solid-liquid interface and plays a key role in determining electrochemical performance. Tracking the spatiotemporal dynamics of the diffusion layer has remained an unresolved challenge. With spatially resolved synchrotron X-ray fluorescence microscopy and micro-X-ray absorption spectroscopy, we demonstrate the in situ visualization and chemical identification of the dynamic diffusion layer near the electrode surface under electrochemical operating conditions. Our method allows for direct mapping of the reactive electrochemical interface and provides insights into engineering the diffusion layer for improving electrochemical performance.

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