The uncontrolled dendrite growth of lithium metal anodes (LMAs) caused by unstable anode/electrolyte interface and uneven lithium deposition have impeded the practical applications of lithium metal batteries (LMBs). Constructing a robust artificial solid electrolyte interphase (SEI) and regulating the lithium deposition behavior is an effective strategy to address these issues. Herein, a three-dimensional (3D) lithium anode with gradient Li₃N has been in-situ fabricated on carbon-based framework by thermal diffusion method (denoted as CC/Li/Li₃N). Density functional theory (DFT) calculations reveal that Li₃N can effectively promote the transport of Li⁺ due to the low energy barrier of Li⁺ diffusion. As expected, the Li₃N-rich conformal artificial SEI film can not only effectively stabilize the interface and avoid parasitic reactions, but also facilitate fast Li⁺ transport across the SEI layer. The anode matrix with uniformly distributed Li₃N can enable homogenous deposition of Li, thus preventing Li dendrite propagation. Benefiting from these merits, the CC/Li/Li₃N anode achieves ultralong-term cycling for >1000 h at a current density of 2 mA cm⁻² and dendrite-free Li deposition at an ultrahigh rate of 20 mA cm⁻². Moreover, the full cells coupled with LiFePO₄ cathodes show extraordinary cycling stability for >300 cycles in liquid-electrolyte-based batteries and display a high-capacity retention of 96.7% after 100 cycles in solid-state cells, demonstrating the promising prospects for the practical applications of LMBs.

由于负极/电解质界面不稳定和锂沉积不均匀导致锂金属负极（LMA）枝晶生长不受控制，阻碍了锂金属电池（LMB）的实际应用。构建稳健的人工固体电解质界面（SEI）并调节锂沉积行为是解决这些问题的有效策略。在此，通过热扩散法（CC/Li/Li ₃ N）在碳基骨架上原位制备了具有梯度Li ₃ N的三维（3D）锂负极。密度泛函理论（DFT）计算表明，由于Li + 的低能垒，Li ³ N_可以有效地促进Li ^+的传输扩散。正如预期的那样，富含Li ₃ N的共形人工SEI膜不仅可以有效地稳定界面并避免寄生反应，还可以促进Li ⁺在SEI层中的快速传输。_{具有均匀分布的Li 3} N的阳极基体可以使Li均匀沉积，从而防止Li枝晶生长。得益于这些优点，CC/Li/Li _{3 N 负极在 2 mA cm} ^-2的电流密度下实现了 >1000 小时的超长期循环，并在 20 mA cm ^-2的超高速率下实现了无枝晶的锂沉积。此外，全电池与 LiFePO ₄正极在液体电解质电池中循环超过 300 次时表现出非凡的循环稳定性，在固态电池中循环 100 次后仍显示出 96.7% 的高容量保持率，这表明 LMB 的实际应用前景广阔。