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Black Phosphorus Degradation during Intercalation and Alloying in Batteries
ACS Nano ( IF 15.8 ) Pub Date : 2023-03-27 , DOI: 10.1021/acsnano.2c08776 Samia Said 1 , Zhenyu Zhang 1, 2 , Rebecca R C Shutt 3 , Hector J Lancaster 3 , Dan J L Brett 1, 2 , Christopher A Howard 3 , Thomas S Miller 1, 2
ACS Nano ( IF 15.8 ) Pub Date : 2023-03-27 , DOI: 10.1021/acsnano.2c08776 Samia Said 1 , Zhenyu Zhang 1, 2 , Rebecca R C Shutt 3 , Hector J Lancaster 3 , Dan J L Brett 1, 2 , Christopher A Howard 3 , Thomas S Miller 1, 2
Affiliation
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Numerous layered materials are being recognized as promising candidates for high-performance alkali-ion battery anodes, but black phosphorus (BP) has received particular attention. This is due to its high specific capacity, due to a mixed alkali-ion storage mechanism (intercalation-alloying), and fast alkali-ion transport within its layers. Unfortunately, BP based batteries are also commonly associated with serious irreversible losses and poor cycling stability. This is known to be linked to alloying, but there is little experimental evidence of the morphological, mechanical, or chemical changes that BP undergoes in operational cells and thus little understanding of the factors that must be mitigated to optimize performance. Here the degradation mechanisms of BP alkali-ion battery anodes are revealed through operando electrochemical atomic force microscopy (EC-AFM) and ex situ spectroscopy. Among other phenomena, BP is observed to wrinkle and deform during intercalation but suffers from complete structural breakdown upon alloying. The solid electrolyte interphase (SEI) is also found to be unstable, nucleating at defects before spreading across the basal planes but then disintegrating upon desodiation, even above alloying potentials. By directly linking these localized phenomena with the whole-cell performance, we can now engineer stabilizing protocols for next-generation high-capacity alkali-ion batteries.
中文翻译：
电池插层合金化过程中黑磷的降解
许多层状材料被认为是高性能碱离子电池阳极的有前途的候选材料，但黑磷 (BP) 受到了特别关注。这是由于其高比容量、混合碱离子存储机制（插层合金化）以及其层内的快速碱离子传输。不幸的是，基于 BP 的电池通常也与严重的不可逆损失和循环稳定性差有关。已知这与合金化有关，但几乎没有实验证据表明 BP 在运行电池中经历的形态、机械或化学变化，因此对必须减轻以优化性能的因素知之甚少。这里通过操作揭示了 BP 碱离子电池阳极的降解机制电化学原子力显微镜 (EC-AFM) 和非原位光谱学。在其他现象中，观察到 BP 在插层过程中起皱和变形，但在合金化时会发生完全结构破坏。还发现固体电解质中间相 (SEI) 不稳定，在扩散到基面之前在缺陷处成核，但随后在脱钠时分解，甚至高于合金化电位。通过将这些局部现象与全电池性能直接联系起来，我们现在可以为下一代高容量碱离子电池设计稳定方案。
更新日期：2023-03-27
中文翻译：
电池插层合金化过程中黑磷的降解
许多层状材料被认为是高性能碱离子电池阳极的有前途的候选材料，但黑磷 (BP) 受到了特别关注。这是由于其高比容量、混合碱离子存储机制（插层合金化）以及其层内的快速碱离子传输。不幸的是，基于 BP 的电池通常也与严重的不可逆损失和循环稳定性差有关。已知这与合金化有关，但几乎没有实验证据表明 BP 在运行电池中经历的形态、机械或化学变化，因此对必须减轻以优化性能的因素知之甚少。这里通过操作揭示了 BP 碱离子电池阳极的降解机制电化学原子力显微镜 (EC-AFM) 和非原位光谱学。在其他现象中，观察到 BP 在插层过程中起皱和变形，但在合金化时会发生完全结构破坏。还发现固体电解质中间相 (SEI) 不稳定，在扩散到基面之前在缺陷处成核，但随后在脱钠时分解，甚至高于合金化电位。通过将这些局部现象与全电池性能直接联系起来，我们现在可以为下一代高容量碱离子电池设计稳定方案。
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