Stabilizing Solid Electrolyte Interphase on Liquid Metal Via Dynamic Hydrogel-Derived Carbon Framework Encapsulation,Advanced Materials

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Stabilizing Solid Electrolyte Interphase on Liquid Metal Via Dynamic Hydrogel-Derived Carbon Framework Encapsulation
Advanced Materials ( IF 27.4 ) Pub Date : 2024-03-23 , DOI: 10.1002/adma.202401234
Hanning Zhang _{1,

2} , Wei Zhang _{1,

2} , Dan Luo ₃ , Siyu Zhang _{1,

2} , Lingqiao Kong _{1,

2} , Huan Xia _{1,

2} , Qian Xie _{1,

2} , Gang Xu _{1,

2} , Zhongwei Chen ₃ , Zhengming Sun _{1,

2}

Affiliation

Eutectic gallium–indium liquid metal (EGaIn-LM), with a considerable capacity and unique self-healing properties derived from its intrinsic liquid nature, gains tremendous attention for lithium-ion batteries (LIBs) anode. However, the fluidity of the LM can trigger continuous consumption of the electrolyte, and its liquid–solid transition during the lithiation/de-lithiation process may result in the rupture of the solid electrolyte interface (SEI). Herein, LM is employed as an initiator to in situ assemble the 3D hydrogel for dynamically encapsulating itself; the LM nanoparticles can be homogeneously confined within the hydrogel-derived carbon framework (HDC) after calcination. Such design effectively alleviates the volume expansion of LM and facilitates electron transportation, resulting in a superior rate capability and long-term cyclability. Further, the “dual-layer” SEI structure and its key components, including the robust LiF outer layer and corrosion-resistant and ionic conductive LiGaO_x inner layer are revealed, confirming the involvement of LM in the formation of SEI, as well as the important role of carbon framework in reducing interfacial side reactions and SEI decomposition. This work provides a distinct perspective for the formation, structural evolution, and composition of SEI at the liquid/solid interface, and demonstrates an effective strategy to construct a reliable matrix for stabilizing the SEI.

中文翻译：

通过动态水凝胶衍生碳框架封装稳定液态金属上的固体电解质界面

共晶镓-铟液态金属（EGaIn-LM）具有相当大的容量和源自其固有液体性质的独特自愈特性，作为锂离子电池（LIB）阳极受到了极大的关注。然而，LM的流动性会引发电解质的持续消耗，并且其在锂化/脱锂过程中的液固转变可能导致固体电解质界面（SEI）的破裂。在此，采用LM作为引发剂原位组装3D水凝胶以动态封装自身；煅烧后，LM 纳米粒子可以均匀地限制在水凝胶衍生的碳框架 (HDC) 内。这种设计有效地缓解了LM的体积膨胀，促进电子传输，从而具有优异的倍率性能和长期循环性能。此外，还揭示了“双层”SEI结构及其关键组件，包括坚固的LiF外层和耐腐蚀且离子导电的LiGaO _x内层，证实了LM参与SEI的形成，以及碳骨架在减少界面副反应和SEI分解方面发挥着重要作用。这项工作为液/固界面处 SEI 的形成、结构演化和组成提供了独特的视角，并展示了构建稳定 SEI 的可靠矩阵的有效策略。

更新日期：2024-03-23

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