The mossy lithium dendrite growth during repeated lithium plating/stripping induces low Coulombic efficiency, poor lifespan, and safety concerns of working lithium metal batteries. Herein, atomically dispersed CoN_x‐doped graphene is exploited as a host to accommodate dendrite‐free lithium deposits. The coordination between Co and N in the conductive matrix can effectively regulate the local electronic structure, and thereby enhance the adsorption of lithium ions and promote the following nucleation process. Meanwhile, the doped N facilitates high dispersion of Co atoms into graphene through the CoN coordination bond. The strong lithiophilicity provided by N coordinated with Co promises a uniform lithium nucleation behavior, further contributing to the smooth lithium deposition morphology. These characteristics afford a superhigh Coulombic efficiency of 99.2% at 2.0 mA cm⁻² (≈400 cycles) and 5.0 mA cm⁻² (350 cycles), and 98.2% at 10.0 mA cm⁻² (200 cycles) with a capacity of 2.0 mAh cm⁻². LiFePO₄|CoNC–Li full cells deliver a long lifespan of 340 cycles at 1.0 C (240 cycles for routine cells). This offers fresh insights into effectively regulating the lithiophilic chemistry of lithium metal host toward uniform nucleation and growth of lithium deposits in working high‐energy‐density batteries.

中文翻译：

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原子分散的Lithiophilic CoNx站点指导的均匀锂成核，以确保锂金属电池安全

在重复的锂电镀/剥离过程中长满苔藓状的锂树枝状晶体会引起库仑效率低，寿命差以及对工作的锂金属电池的安全性问题。在本文中，原子分散的CoN _x掺杂石墨烯被用作主体，以容纳无枝晶的锂沉积物。导电基体中Co和N之间的配位可以有效地调节局部电子结构，从而增强锂离子的吸附并促进随后的成核过程。同时，掺杂N促进Co原子的高分散到通过联合石墨烯N配位键。N与Co配合提供的强大的亲硫性保证了均匀的锂成核行为，进一步有助于平滑的锂沉积形态。这些特性在2.0 mA cm ^-2（≈400个循环）和5.0 mA cm ^-2（350个循环）下提供99.2％的超高库仑效率，在10.0 mA cm ^-2（200个循环）下具有98.2％的超高库仑效率。mAh cm ^-2。LiFePO ₄ | CoNC-Li充满电的电池在1.0 C时可提供340个循环的长寿命（常规电池为240个循环）。这为有效调节锂金属主体的亲硫化学，以使工作的高能量密度电池中的锂沉积物均匀成核和生长提供了新的见解。