Regulating the surface structure of the collector to synergistically reduce the nucleation and lateral growth barrier of Li⁺ electrodeposition is key to long-cycle anode-free Li-metal batteries (AFLMB), but its adjusting mechanism and modulation remain a formidable challenge. Herein, a previously unreported heterogeneous collector with hard-base sites and soft-acid sites is proposed to enhance chemical interaction with hard-acid Li⁺ and soft-base Li atoms, respectively. Theoretical analysis demonstrates that the addition of Co single atoms into the N–C host improves the hardness of N bases and the softness of the carbon matrix. According to the results of operando microscopy and electrochemical measurement, the HBSA-Co SA collector with controlled local chemical softness substantially reduces nucleation/growth barriers without any dendrite morphology. The NCM811-based Li metal cells with a high cathode area capacity of 15 mA h cm⁻² and limited lithium excess achieve a superior capacity retention rate of 98.8% after 150 cycles. This finding provides an avenue to rationally design a highly efficient collector for AFLMB.

中文翻译：

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调节集电极的局部化学软度，使无阳极锂金属电池的锂沉积均匀化


调节集电极的表面结构以协同减少 Li⁺ 电沉积的成核和横向生长势垒是长周期无负极锂金属电池 （AFLMB） 的关键，但其调节机制和调制仍然是一个艰巨的挑战。在此，提出了一种以前未报道的具有硬碱位点和软酸位点的非均相捕集剂，以分别增强与硬酸 Li⁺ 和软碱 Li 原子的化学相互作用。理论分析表明，在 N-C 主体中添加 Co 单原子可以提高 N 碱的硬度和碳基体的柔软度。根据原位显微镜和电化学测量的结果，具有受控局部化学柔软度的 HBSA-Co SA 捕收剂大大减少了成核/生长障碍，而没有任何枝晶形态。基于 NCM811 的锂金属电池具有 15 mA h ^cm-2 的高阴极面积容量和有限的锂过量，在 150 次循环后实现了 98.8% 的优异容量保持率。这一发现为合理地为 AFLMB 设计高效的收集器提供了一条途径。