Enhancing the electrochemical stability of lithium anode by introducing lithiophilic three-dimensional framework Li2Cu3Zn

As we all known, the most promising alternative anode for the next-generation energy storage devices is the lithium metal anode. But the unpredictable dendrite growth and volume expansion during the cycles impedes its applications and commercialization. The Li-Cu-Zn three-phases alloy materials (including Li2Cu3Zn, Li-Zn and Li) have been synthesized to solve these problems. According to the density functional theory (DFT) analysis, all results indicate that the Li2Cu3Zn ternary alloy has the higher absorption energy of Li than bare Li, suggesting the superior lithiophilic. Meanwhile, the construction of Li2Cu3Zn alloy 3D skeleton is beneficial to uniform the Li+ flux and reducing the local current density. Furthermore, based on the analysis of in-situ X-ray diffraction, Li2Cu3Zn skeleton can keep stable during the cycles. The Li-Cu-Zn electrodes exhibit the stable cycling performance about more than 1200 h and pure lithium only for about 120 h (at 1 mA cm−2 and 1 mAh cm−2). And at 0.5 C, after 100 cycles, the NCM811 (LiNi0.8Co0.1Mn0.1O2) ||Li-Cu-Zn cell delivers an excellent cycling stability for 92.3% capacity retention. In this work, uniform deintercalation of lithium ions through three-dimensional alloy framework structure provides a research basis for lithium-free anodes.