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

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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在像差校正环境透射电子显微镜中对高温下 Li-CO2 纳米电池的电化学反应进行原位成像

DOI:
10.1007/s12274-021-3514-9
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发表时间:
2021-05
期刊:
影响因子:
9.9
通讯作者:
Huang Jianyu
Huang Jianyu
中科院分区:
材料科学1区
文献类型:
--
作者:
Jia Peng;Yu Meiqi;Zhang Xuedong;Yang Tingting;Zhu Dingding;Shen Tongde;Zhang Liqiang;Tang Yongfu;Huang Jianyu

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可充锂-二氧化碳(Li-CO2)电池由于其高的理论能量密度和捕获CO2的能力而受到广泛关注。然而,锂-CO2电池的电化学反应机理,特别是放电产物Li 2CO 3的分解机理尚不清楚,阻碍了其实际应用。研究Li 2CO 3的电化学性质是提高Li-CO2电池性能的关键。本文采用原位环境透射电子显微镜(ETEM)技术研究了Li-CO2电池中Li 2CO 3在充放电过程中的电化学行为。在放电过程中,Li 2CO 3在碳纳米管(CNTs)和银纳米线(Ag NWs)等阴极介质表面成核聚集,但在室温下充电过程中难以分解。为了促进Li 2CO 3的分解,在高温下进行充电反应,在此期间Li 2CO 3分解为锂并释放气体。密度泛函理论(DFT)计算表明,温度和偏压的协同效应促进了Li 2CO 3的分解。本研究不仅为高温Li-CO2纳米电池的研究提供了一个基础性的认识,同时也提供了一种有效的技术,在高温下放电/充电,以提高锂-二氧化碳电池的可循环性的能量存储应用。
Rechargeable lithium-carbon dioxide (Li-CO 2 ) batteries have attracted much attention due to their high theoretical energy densities and capture of CO 2 . However, the electrochemical reaction mechanisms of rechargeable Li-CO 2 batteries, particularly the decomposition mechanisms of the discharge product Li 2 CO 3 are still unclear, impeding their practical applications. Exploring electrochemistry of Li 2 CO 3 is critical for improving the performance of Li-CO 2 batteries. Herein, in-situ environmental transmission electron microscopy (ETEM) technique was used to study electrochemistry of Li 2 CO 3 in Li-CO 2 batteries during discharge and charge processes. During discharge, Li 2 CO 3 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 Li 2 CO 3 , the charge reactions were conducted at high temperatures, during which Li 2 CO 3 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 Li 2 CO 3 . This study not only provides a fundamental understanding to the high temperature Li-CO 2 nanobatteries, but also offers a valid technique, i.e., discharging/charging at high temperatures, to improve the cyclability of Li-CO 2 batteries for energy storage applications.
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