Lithium metal batteries are considered as high energy density battery systems with very promising prospects and have been widely studied. However, The uncontrollable plating/stripping behavior, infinite volume change and dendrites formation of lithium metal anode restrict the application. The uncontrolled nucleation of lithium caused by the nonuniform multi-physical field distributions, can lead to the undesirable lithium deposition. Herein, a graphene composite uniformly loaded with Ag nano-particles (Ag NPs) is prepared through a facile Gamma ray irradiation method and assembled into self-supported film with layered structure (Ag-rGO film). When such film is used as a lithium metal anode host, the uncontrolled deposition is converted into a highly nucleation-induced process. On one hand, the Ag NPs distributed between the interlayers of graphene can preferentially induce lithium nucleation and enable uniform deposition morphology of lithium between interlayers. On the other hand, the stable layered graphene structure can accommodate volume change, stabilize the interface between anode and electrolyte and inhibit dendrites formation. Therefore, the layered Ag-rGO film as anode host can reach a high Coulombic efficiency over 93.3% for 200 cycle (786 h) at a current density of 1 mA cm⁻² for 2 mAh cm⁻² in carbonate-based electrolyte. This work proposes a facile Gamma ray irradiation method to prepare metal/3D-skeleton structure as lithium anode host and demonstrates the potential to regulate the lithium metal deposition behaviors via manipulating the distribution of lithiophilic metal (e.g. Ag) in 3D frameworks. This may offer a practicable thinking for the subsequent design of the lithium metal anode.

锂金属电池被认为是具有非常有前途的前景的高能量密度电池系统，并且已经被广泛研究。然而，不可控制的电镀/剥离行为，无限的体积变化和锂金属阳极的枝晶形成限制了该应用。由不均匀的多物理场分布引起的锂不受控制的成核，可能导致不良的锂沉积。在此，通过简便的伽马射线辐照法制备均匀地负载有Ag纳米粒子（Ag NPs）的石墨烯复合材料，并将其组装成具有层状结构的自支撑膜（Ag-rGO膜）。当这种膜用作锂金属阳极主体时，不受控制的沉积转化为高度成核诱导的过程。一方面，分布在石墨烯夹层之间的Ag NPs可以优先诱导锂成核，并使锂在夹层之间具有均匀的沉积形态。另一方面，稳定的层状石墨烯结构可以适应体积变化，稳定阳极和电解质之间的界面并抑制树枝状晶体的形成。因此，在电流密度为1 mA cm的情况下，在200个循环（786小时）内，作为阳极主体的层状Ag-rGO薄膜可以达到93.3％的高库仑效率。^-2 2毫安厘米^-2在基于碳酸酯的电解液。这项工作提出了一种简便的伽马射线辐照方法，以制备金属/ 3D骨架结构作为锂阳极主体，并证明了通过操纵3D框架中亲硫金属（例如Ag）的分布来调节锂金属沉积行为的潜力。这可以为锂金属阳极的后续设计提供实用的思路。