Nanoscale Visualization of Reversible Redox Pathways in Lithium-Sulfur Battery Using In Situ AFM-SECM
Nanoscale Visualization of Reversible Redox Pathways in Lithium-Sulfur Battery Using In Situ AFM-SECM
复制标题
使用原位 AFM-SECM 实现锂硫电池中可逆氧化还原途径的纳米级可视化
DOI：
10.1149/1945-7111/ac70ff
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发表时间：
2022
影响因子：
3.9
通讯作者：
Arava, Leela Mohana
中科院分区：
文献类型：
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作者：
Thangavel, Naresh Kumar;Mahankali, Kiran;Arava, Leela Mohana
推导中间体的电化学活性并提供材料溶液以改变其反应途径是开发先进储能系统（如锂硫（Li-S）电池）的关键。在这里，我们提供了基板引导的反应途径的中间多硫化物和它们的相关性的放电最终产品的氧化还原活性的机制的观点，使用原位原子力显微镜为基础的扫描电化学显微镜（AFM-SECM）耦合拉曼光谱在纳米级的时空分辨率。原位SECM中间产物检测沿着以及电极/电解质界面处的拉曼分析表明，Li 2 S的沉淀可以通过电化学活性二硫化锂（Li 2 S2）中间步骤发生。通过详细的光谱电化学和形态学映射，我们解释了衬底依赖的Li 2 S 2形成对后续循环中的Li 2 S氧化产生不利影响，从而降低了电池的往返效率和整体性能。本研究提供了有关锂硫电池中多硫反应途径的纳米级解析信息，涉及电极结构及其性能。
Deducing the electrochemical activity of intermediates and providing materials solution to alter their reaction pathways holds the key for developing advanced energy storage systems such as lithium-sulfur (Li-S) batteries. Herein, we provide mechanistic perspectives of the substrate guided reaction pathways of intermediate polysulfides and their correlation to the redox activity of discharge end products using In Situ atomic force microscopy-based scanning electrochemical microscopy (AFM-SECM) coupled Raman spectroscopy at nanoscale spatiotemporal resolution. In Situ SECM intermediate detection along with Raman analysis at the electrode/electrolyte interface reveals that the precipitation of Li 2 S can occur via an electrochemically active lithium disulfide (Li 2 S 2) intermediate step. With a detailed spectro-electrochemical and morphological mapping, we decipher that the substrate-dependent Li 2 S 2 formation adversely affects the Li 2 S oxidation in the subsequent cycles, thereby reducing the round-trip efficiency and overall performance of the cell. The present study provides nanoscale-resolved information regarding the polysulfide reaction pathways in Li-S batteries with respect to the electrode structure and its properties.