反钙钛矿Li$_2$Fe)SO中阳离子与阴离子氧化还原活性的分离
Separating cationic and anionic redox activity in antiperovskite Li$_2$Fe)SO
AI总结：
本研究通过分离反钙钛矿Li$_2$Fe)SO中的阳离子与阴离子氧化还原过程，发现阴离子过程导致循环稳定性差，仅利用阳离子过程可实现超100次稳定循环，为提升电化学储能性能提供了途径。
摘要：
由于同时存在阳离子和阴离子氧化还原活性，富锂反钙钛矿有望成为极具吸引力的高容量正极材料。然而，关于将电化学阳离子过程与阴离子过程分离的效果及其对电化学性能的相关影响，人们知之甚少。在此背景下，我们报告了三种不同Li$_2$Fe)SO材料这一示例的电化学性能，重点在于分离阳离子与阴离子效应。通过高压阴离子过程，最初可达到约400~mAh/g的惊人电化学容量。然而，我们的结果确定阴离子过程是循环稳定性差的原因，并证明通过仅限制在阳离子过程，可以避免先前文献中报道的容量衰减。沿着这一路径，我们的Li$_2$Fe)SO-BM500表现出显著改善的性能，表现为在1~C下容量约为175~mAh/g时，超过100次循环的恒定电化学循环。我们的方法还允许我们研究裸反钙钛矿相的电化学性能，排除了来自初始或循环引起的杂质相的外在活性。我们的结果强调，合成条件是富锂反钙钛矿电化学性能的关键决定因素，特别是关于电化学二次相的数量，而粒径未被发现是关键参数。总体而言，分离和理解富锂反钙钛矿中阳离子与阴离子氧化还原活性的影响，为进一步提升其在电化学储能中的性能提供了途径。
英文摘要：
Lithium-rich antiperovskite promise to be a compelling high-capacity cathode material due to existence of both cationic and anionic redox activity. Little is however known about the effect of separating the electrochemical cationic from the anionic process and the associated implications on the electrochemical performance. In this context, we report the electrochemical properties of the illustrative example of three different Li$_2$Fe)SO materials with a focus on separating cationic from anionic effects. With the high voltage anionic process, an astonishing electrochemical capacity of around 400~mAh/g can initially be reached. Our results however identify the anionic process as the cause of poor cycling stability and demonstrate that fading reported in previous literature is avoided by restricting to only the cationic processes. Following this path, our Li$_2$Fe)SO-BM500 shows strongly improved performance indicated by constant electrochemical cycling over 100 cycles at a capacity of around 175~mAh/g at 1~C. Our approach also allows us to investigate the electrochemical performance of the bare antiperovskite phase excluding extrinsic activity from initial or cycling-induced impurity phases. Our results underscore that synthesis conditions are a critical determinant of electrochemical performance in lithium-rich antiperovskites, especially with regard to the amount of electrochemical secondary phases, while the particle size has not been found a crucial parameter. Overall, separating and understanding the effects of cationic from anionic redox activity in lithium-rich antiperovskites provides the route to further improve their performance in electrochemical energy storage.
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