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Research Article

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

Peng Jia1,§, Meiqi Yu1,3,§, Xuedong Zhang2, Tingting Yang1, Dingding Zhu2, Tongde Shen1, Liqiang Zhang1( ), Yongfu Tang1,3, Jianyu Huang1,2
Clean Nano Energy Center State Key Laboratory of Metastable Materials Science and Technology Yanshan University Qinhuangdao 066004 China
Key Laboratory of Low Dimensional Materials and Application Technology of Ministry of Education School of Materials Science and Engineering Xiangtan University Xiangtan 411105 China
Hebei Key Laboratory of Applied Chemistry College of Environmental and Chemical Engineering Yanshan University Qinhuangdao 066004 China

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

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Graphical Abstract

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.

Keywords

in-situ environmental transmission electron microscopyhigh temperature Li-CO2 nanobatterieselectrochemistryLi2CO3

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Nano Research
Volume 15 Issue 1,
January 2022
Pages 542-550
DOI: 10.1007/s12274-021-3514-9
Cite this article:
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 Research, 2022, 15(1): 542-550. https://doi.org/10.1007/s12274-021-3514-9
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Received: 29 January 2021
Revised: 23 March 2021
Accepted: 11 April 2021
Published: 04 May 2021
© Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2021
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