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Tailoring Breathing Behavior of Solid Electrolyte Interphases Unraveled by Cryogenic Transmission Electron Microscopy
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2023-04-07 , DOI: 10.1002/aenm.202300240 Xuyun Guo 1, 2 , Xiaoqiong Du 1, 2 , Valeria Nicolosi 2 , Biao Zhang 1 , Ye Zhu 1
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2023-04-07 , DOI: 10.1002/aenm.202300240 Xuyun Guo 1, 2 , Xiaoqiong Du 1, 2 , Valeria Nicolosi 2 , Biao Zhang 1 , Ye Zhu 1
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The cycling stability of batteries is closely related to the dynamic evolution of solid electrolyte interphases (SEIs) in response to the discharging/charging processes. Here, the state-of-the-art cryogenic transmission electron microscopy (cryo-TEM) and spectroscopy are utilized to probe the SEI breathing behavior induced by discharging/charging on the conversion-type anode made of Fe2O3 quasi-cubes. The incorporation of the identical-location strategy allows the tracking of the evolution of the same SEIs at different charge states. SEI breathing is shown to involve swelling (contracting) upon lithiation (de-lithiation) driven by the reversible compositional change. Bare Fe2O3 anodes develop an unstable SEI layer due to the intermixing with the lithiation product Li2O, which exhibits a large thickness variation upon breathing as well as excessive growth. A transition from organic to inorganic-type SEI is also identified upon cycling, which gives rise to significantly increased SEI resistance. To tailor the SEI behavior, N-doped carbon coating is applied on Fe2O3 (Fe2O3@CN), which can effectively separate the lithiation product from SEI. A thinner and chemically more stable SEI layer develops on Fe2O3@CN, resulting in remarkably enhanced cycling stability compared to bare Fe2O3. This work demonstrates the importance of understanding and optimizing the dynamic behavior of SEIs to achieve better battery performance.
中文翻译：
低温透射电子显微镜揭示固体电解质界面的调整呼吸行为
电池的循环稳定性与响应放电/充电过程的固体电解质界面（SEI）的动态演变密切相关。在这里，最先进的低温透射电子显微镜 (cryo-TEM) 和光谱学用于探测由 Fe 2 O 3 准立方体制成的转换型阳极上放电/充电引起的SEI呼吸行为。相同位置策略的结合允许跟踪相同 SEI 在不同电荷状态下的演变。SEI 呼吸显示涉及由可逆成分变化驱动的锂化（脱锂）时的膨胀（收缩）。裸Fe 2 O 3由于与锂化产物 Li 2 O 混合，阳极会形成不稳定的 SEI 层，其在呼吸时表现出较大的厚度变化以及过度生长。在循环过程中还发现了从有机型到无机型 SEI 的转变，这导致 SEI 阻力显着增加。为了定制 SEI 行为，在 Fe 2 O 3 (Fe 2 O 3 @CN)上应用了 N 掺杂碳涂层，这可以有效地将锂化产物与 SEI 分离。在 Fe 2 O 3 @CN上形成更薄且化学更稳定的 SEI 层，与裸露的 Fe 2 O 3相比，循环稳定性显着增强. 这项工作证明了理解和优化 SEI 的动态行为以获得更好的电池性能的重要性。
更新日期：2023-04-07
中文翻译：
低温透射电子显微镜揭示固体电解质界面的调整呼吸行为
电池的循环稳定性与响应放电/充电过程的固体电解质界面（SEI）的动态演变密切相关。在这里，最先进的低温透射电子显微镜 (cryo-TEM) 和光谱学用于探测由 Fe 2 O 3 准立方体制成的转换型阳极上放电/充电引起的SEI呼吸行为。相同位置策略的结合允许跟踪相同 SEI 在不同电荷状态下的演变。SEI 呼吸显示涉及由可逆成分变化驱动的锂化（脱锂）时的膨胀（收缩）。裸Fe 2 O 3由于与锂化产物 Li 2 O 混合，阳极会形成不稳定的 SEI 层，其在呼吸时表现出较大的厚度变化以及过度生长。在循环过程中还发现了从有机型到无机型 SEI 的转变，这导致 SEI 阻力显着增加。为了定制 SEI 行为，在 Fe 2 O 3 (Fe 2 O 3 @CN)上应用了 N 掺杂碳涂层，这可以有效地将锂化产物与 SEI 分离。在 Fe 2 O 3 @CN上形成更薄且化学更稳定的 SEI 层，与裸露的 Fe 2 O 3相比，循环稳定性显着增强. 这项工作证明了理解和优化 SEI 的动态行为以获得更好的电池性能的重要性。
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