Lithium (Li) metal is promising for high energy density batteries due to its low electrochemical potential (−3.04 V) and high specific capacity (3860 mAh g⁻¹). However, the safety issues impede the commercialization of Li anode batteries. In this work, research of hierarchical structure designs for Li anodes to suppress Li dendrite growth and alleviate volume expansion from the interior (by the 3D current collector and host matrix) to the exterior (by the artificial solid electrolyte interphase (SEI), protective layer, separator, and solid state electrolyte) is concluded. The basic principles for achieving Li dendrite and volume expansion free Li anode are summarized. Following these principles, 3D porous current collector and host matrix are designed to suppress the Li dendrite growth from the interior. Second, artificial SEI, the protective layer, and separator as well as solid‐state electrolyte are constructed to regulate the distribution of current and control the Li nucleation and deposition homogeneously for suppressing the Li dendrite growth from exterior of Li anode. Ultimately, this work puts forward that it is significant to combine the Li dendrite suppression strategies from the interior to exterior by 3D hierarchical structure designs and Li metal modification to achieve excellent cycling and safety performance of Li metal batteries.

中文翻译：

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分层结构设计从内部到外部的锂枝晶抑制策略研究进展。

锂（Li）金属具有低电化学势（-3.04 V）和高比容量（3860 mAh g ^-1），因此有望用于高能量密度电池）。然而，安全问题阻碍了锂阳极电池的商业化。在这项工作中，研究了锂阳极的分层结构设计，以抑制锂枝晶生长并减轻从内部（通过3D集电器和主体基质）到外部（通过人工固体电解质中间相（SEI），保护层）的体积膨胀，隔板和固态电解质）。总结了实现锂枝晶和无体积膨胀锂阳极的基本原理。遵循这些原理，设计了3D多孔集电器和基质，以抑制Li树枝状晶体从内部生长。第二，人造SEI，保护层，构造隔板和固态电解质以调节电流分布，并均匀地控制Li成核和沉积，从而抑制Li枝晶从Li阳极外部生长。最终，这项工作提出，通过3D分层结构设计和锂金属改性相结合，从内部到外部抑制锂枝晶的策略，对于实现锂金属电池出色的循环性能和安全性具有重要意义。