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In-situ imaging the electrochemical reactions of Li-CO2 nanobatteries at high temperatures in an aberration corrected environmental transmission electron microscope

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Abstract

Rechargeable lithium-carbon dioxide (Li-CO2) batteries have attracted much attention due to their high theoretical energy densities and capture of CO2. However, the electrochemical reaction mechanisms of rechargeable Li-CO2 batteries, particularly the decomposition mechanisms of the discharge product Li2CO3 are still unclear, impeding their practical applications. Exploring electrochemistry of Li2CO3 is critical for improving the performance of Li-CO2 batteries. Herein, in-situ environmental transmission electron microscopy (ETEM) technique was used to study electrochemistry of Li2CO3 in Li-CO2 batteries during discharge and charge processes. During discharge, Li2CO3 was nucleated and accumulated on the surface of the cathode media such as carbon nanotubes (CNTs) and Ag nanowires (Ag NWs), but it was hard to decompose during charging at room temperature. To promote the decomposition of Li2CO3, the charge reactions were conducted at high temperatures, during which Li2CO3 was decomposed to lithium with release of gases. Density functional theory (DFT) calculations revealed that the synergistic effect of temperature and biasing facilitates the decomposition of Li2CO3. This study not only provides a fundamental understanding to the high temperature Li-CO2 nanobatteries, but also offers a valid technique, i.e., discharging/charging at high temperatures, to improve the cyclability of Li-CO2 batteries for energy storage applications.

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Acknowldgements

This work was financially supported by the the National Natural Science Foundation of China (Nos. 52022088, 51971245, 51772262, 21406191, U20A20336, and 21935009), Bei**g Natural Science Foundation (No. 2202046), Selective funding for provincial postdoctoral research projects (No. B2019003018), Fok Ying-Tong Education Foundation of China (No. 171064), Natural Science Foundation of Hebei Province (Nos. B2020203037, and B2018203297), and Hunan Innovation Team (No. 2018RS3091).

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  1. Peng Jia and Meiqi Yu contributed equally to this work.

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  1. Clean Nano Energy Center, State Key Laboratory of Metastable Materials Science and Technology, Yanshan University, Qinhuangdao, 066004, China

    Peng Jia, Meiqi Yu, Tingting Yang, Tongde Shen, Liqiang Zhang, Yongfu Tang & Jianyu Huang

  2. Key Laboratory of Low Dimensional Materials and Application Technology of Ministry of Education, School of Materials Science and Engineering, **angtan University, **angtan, 411105, China

    Xuedong Zhang, Dingding Zhu & Jianyu Huang

  3. Hebei Key Laboratory of Applied Chemistry, College of Environmental and Chemical Engineering, Yanshan University, Qinhuangdao, 066004, China

    Meiqi Yu & Yongfu Tang

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In-situ imaging the electrochemical reactions of Li-CO2 nanobatteries at high temperatures in an aberration corrected environmental transmission electron microscope

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Jia, P., Yu, M., Zhang, X. et al. In-situ imaging the electrochemical reactions of Li-CO2 nanobatteries at high temperatures in an aberration corrected environmental transmission electron microscope. Nano Res. 15, 542–550 (2022). https://doi.org/10.1007/s12274-021-3514-9

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