Topotactic Transformation of Surface Structure Enabling Direct Regeneration of Spent Lithium-Ion Battery Cathodes,Journal of the American Chemical Society

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Topotactic Transformation of Surface Structure Enabling Direct Regeneration of Spent Lithium-Ion Battery Cathodes
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2023-03-06 , DOI: 10.1021/jacs.2c13151
Kai Jia _{1,

2} , Junxiong Wang _{1,

2} , Zhaofeng Zhuang ₁ , Zhihong Piao ₁ , Mengtian Zhang ₁ , Zheng Liang ₂ , Guanjun Ji _{1,

2} , Jun Ma ₁ , Haocheng Ji ₁ , Wenjiao Yao ₃ , Guangmin Zhou ₁ , Hui-Ming Cheng _{4,

5}

Affiliation

Recycling spent lithium-ion batteries (LIBs) has become an urgent task to address the issues of resource shortage and potential environmental pollution. However, direct recycling of the spent LiNi_0.5Co_0.2Mn_0.3O₂ (NCM523) cathode is challenging because the strong electrostatic repulsion from a transition metal octahedron in the lithium layer provided by the rock salt/spinel phase that is formed on the surface of the cycled cathode severely disrupts Li⁺ transport, which restrains lithium replenishment during regeneration, resulting in the regenerated cathode with inferior capacity and cycling performance. Here, we propose the topotactic transformation of the stable rock salt/spinel phase into Ni_0.5Co_0.2Mn_0.3(OH)₂ and then back to the NCM523 cathode. As a result, a topotactic relithiation reaction with low migration barriers occurs with facile Li⁺ transport in a channel (from one octahedral site to another, passing through a tetrahedral intermediate) with weakened electrostatic repulsion, which greatly improves lithium replenishment during regeneration. In addition, the proposed method can be extended to repair spent NCM523 black mass, spent LiNi_0.6Co_0.2Mn_0.2O₂, and spent LiCoO₂ cathodes, whose electrochemical performance after regeneration is comparable to that of the commercial pristine cathodes. This work demonstrates a fast topotactic relithiation process during regeneration by modifying Li⁺ transport channels, providing a unique perspective on the regeneration of spent LIB cathodes.

中文翻译：

表面结构的拓扑转化使废锂离子电池阴极能够直接再生

回收废旧锂离子电池（LIBs）已成为解决资源短缺和潜在环境污染问题的紧迫任务。然而，直接回收用过的 LiNi _0.5 Co _0.2 Mn _0.3 O ₂ (NCM523) 正极具有挑战性，因为锂层中的过渡金属八面体具有强烈的静电排斥力，该八面体由锂层表面形成的岩盐/尖晶石相提供循环后的正极严重破坏了Li ⁺的传输，限制了再生过程中锂的补充，导致再生正极的容量和循环性能较差。在这里，我们提出将稳定的岩盐/尖晶石相拓扑转化为 Ni_0.5 Co _0.2 Mn _0.3 (OH) ₂然后回到NCM523阴极。因此，在静电排斥减弱的通道中（从一个八面体位点到另一个八面体位点，通过四面体中间位点），发生了具有低迁移势垒的局部规整再锂化反应^，这极大地改善了再生过程中的锂补充。此外，所提出的方法可以扩展到修复用过的 NCM523 黑色物质、用过的 LiNi _0.6 Co _0.2 Mn _0.2 O ₂和用过的 LiCoO ₂阴极，其再生后的电化学性能可与商业原始阴极相媲美。^{这项工作通过修改 Li +}传输通道展示了再生过程中的快速拓扑再锂化过程，为废 LIB 正极的再生提供了独特的视角。

更新日期：2023-03-06

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