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Creators/Authors contains: "Zheng, Hongkui"

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  1. Abstract

    Garnet‐type Li7La3Zr2O12(LLZO) solid‐state electrolytes hold great promise for the next‐generation all‐solid‐state batteries. An in‐depth understanding of the phase transformation during synthetic processes is required for better control of the crystallinity and improvement of the ionic conductivity of LLZO. Herein, the phase transformation pathways and the associated surface amorphization are comparatively investigated during the sol–gel and solid‐state syntheses of LLZO using in situ heating transmission electron microscopy (TEM). The combined ex situ X‐ray diffraction and in situ TEM techniques are used to reveal two distinct phase transformation pathways (precursors → La2Zr2O7 → LLZO and precursors → LLZO) and the subsequent layer‐by‐layer crystal growth of LLZO on the atomic scale. It is also demonstrated that the surface amorphization surrounding the LLZO crystals is sensitive to the postsynthesis cooling rate and significantly affects the ionic conductivity of pelletized LLZO. This work brings up a critical but often overlooked issue that may greatly exacerbate the Li‐ion conductivity by undesired synthetic conditions, which can be leveraged to ameliorate the overall crystallinity to improve the electrochemical performance of LLZO. These findings also shed light on the significance of optimizing surface structure to ensure superior performance of Li‐ion conductors.

     
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  4. Abstract

    Conversion‐type materials have been considered as potentially high‐energy‐density alternatives to commercially dominant intercalation‐based electrodes for rechargeable ion batteries and have attracted tremendous research effort to meet the performance for viable energy‐storage technologies. In situ transmission electron microscopy (TEM) has been extensively employed to provide mechanistic insights into understanding the behavior of battery materials. Noticeably, a great portion of previous in situ TEM studies has been focused on conversion‐type materials, but a dedicated review for this group of materials is missing in the literature. Herein, recent developments of in situ TEM techniques for investigation of dynamic phase transformation and associated structural, morphological, and chemical evolutions during conversion reactions with alkali ions in secondary batteries are comprehensively summarized. The materials of interest broadly cover metal oxides, chalcogenides, fluorides, phosphides, nitrides, and silicates with specific emphasis on spinel metal oxides and recently emerged 2D metal chalcogenides. Special focus is placed on the scientific findings that are uniquely obtained by in situ TEM to address fundamental questions and practical issues regarding phase transformation, structural evolution, electrochemical redox, reaction mechanism, kinetics, and degradation. Critical challenges and perspectives are discussed for advancing new knowledge that can bridge the gap between prototype materials and real‐world applications.

     
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