Lithium (Li) metal has attracted significant attention as next‐generation anode material owing to its high theoretical specific capacity and low potential. For enabling the practical application of Li‐metal as an anode according to energy demands, suppressing dendrite growth by controlling the Li‐ion (Li⁺) is crucial. In this study, metal–organic frameworks comprising bipyridinic nitrogen linker (M‐bpyN) are proposed as 3‐dimensional (3D) Li guiding matrix. The proposed approach creates ordered electronegative functional sites that enable the preoccupied Li⁺ in the ordered bipyridine sites to produce isotropic Li growth. The Li guiding matrix containing 3D ordered bipyridinic N sites introduces preoccupied Li⁺ sites that attract the Li growth direction, thereby suppressing the dendrite growth during the electrodeposition of Li. After applying the M‐bpyN layers, stable lifespan of up to 900 cycles in the Li|M‐bpyN|Cu cell and over 1500 h of operation in the Li|M‐bpyN|Li symmetric cell is achieved. Moreover, the Li|M‐bpyN|LiFePO₄ configuration shows a long cycle retention of 350 cycles at 0.5 C. These results indicate that an M‐bpyN Li guiding matrix, which enables a uniform Li⁺ flux by 3D ordered Li⁺‐chelating sites, serve as a suitable host for Li⁺ and enhance the performance of Li‐metal electrodes.

中文翻译：

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用于高性能锂金属电池的有序氮螯合锂离子的高效锂生长控制

锂（Li）金属由于其高理论比容量和低电势而作为下一代负极材料引起了广泛关注。为了根据能源需求实现锂金属作为阳极的实际应用，通过控制锂离子（Li ⁺）来抑制枝晶生长至关重要。在这项研究中，提出了包含联吡啶氮连接体（M-bpyN）的金属有机骨架作为3维（3D）Li引导基质。所提出的方法创建了有序的负电性功能位点，使有序联吡啶位点中占据的Li ⁺能够产生各向同性的Li生长。含有3D有序联吡啶N位点的Li引导基质引入了吸引Li生长方向的占据的Li ⁺位点，从而抑制了Li电沉积过程中的枝晶生长。应用 M-bpyN 层后，Li|M-bpyN|Cu 电池可实现高达 900 个循环的稳定寿命，而 Li|M-bpyN|Li 对称电池可实现超过 1500 小时的运行。此外，Li|M-bpyN|LiFePO ₄构型在 0.5 C 下表现出 350 个循环的长循环保持力。这些结果表明，M-bpyN Li 引导基质可通过 3D 有序 Li ⁺螯合实现均匀的 Li ⁺通量位点，作为 Li ⁺的合适主体并增强锂金属电极的性能。