Injection of oxygen vacancies in the bulk lattice of layered cathodes
Injection of oxygen vacancies in the bulk lattice of layered cathodes
复制标题
在层状阴极体晶格中注入氧空位
DOI：
10.1038/s41565-019-0428-8
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发表时间：
2019-04
影响因子：
38.3
通讯作者：
Zhen-Kun Tang
中科院分区：
文献类型：
--
作者：
Pengfei Yan;Jianming Zheng;Zhen-Kun Tang
表面、界面和晶界通常被认为是大块晶格中产生的缺陷的汇。在这里，我们报道了一种相反的情况，即在粒子表面产生的缺陷被连续泵浦到大块晶格中。我们发现，在充电电池运行过程中，在富锂层状正极粒子表面产生的氧空位向内部晶格迁移。这一过程与激活阴离子氧化还原过程的高截止电压有关。第一性原理计算表明，这种氧化还原过程的触发导致氧空位的形成能和氧化氧离子的迁移势垒急剧降低，从而使氧空位能够迁移到阴极的体晶格中。这项工作揭示了在设计高压锂离子电池高容量层状正极材料时需要考虑的耦合氧化还原动力学。
Surfaces, interfaces and grain boundaries are classically known to be sinks of defects generated within the bulk lattice. Here, we report an inverse case by which the defects generated at the particle surface are continuously pumped into the bulk lattice. We show that, during operation of a rechargeable battery, oxygen vacancies produced at the surfaces of lithium-rich layered cathode particles migrate towards the inside lattice. This process is associated with a high cutoff voltage at which an anionic redox process is activated. First-principle calculations reveal that triggering of this redox process leads to a sharp decrease of both the formation energy of oxygen vacancies and the migration barrier of oxidized oxide ions, therefore enabling the migration of oxygen vacancies into the bulk lattice of the cathode. This work unveils a coupled redox dynamic that needs to be taken into account when designing high-capacity layered cathode materials for high-voltage lithium-ion batteries.
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