Lithium-aluminum layered double hydroxides (LiAl-LDH) have been be successfully applied in commercial-scale for lithium extraction from salt lake brine, however, further advancement of their applications is hampered by suboptimal Li+ adsorption performance and ambiguous extraction process. Herein, a doping engineering strategy was developed to fabricate novel Zn²⁺-doped LiAl-LDH (LiZnAl-LDH) with remarkable higher Li⁺ adsorption capacity (13.4 mg/g) and selectivity (separation factors of 213, 834, 171 for Li⁺/K⁺, Li⁺/Na⁺, Li⁺/Mg²⁺, respectively), as well as lossless reusability in Luobupo brine compared to the pristine LiAl-LDH. Further, combining experiments and simulation calculations, it was revealed that the specific surface area, hydrophilic, and surface attraction for Li⁺ of LiZnAl-LDH were significantly improved, reducing the adsorption energy (E_ad) and Gibbs free energy (ΔG), thus facilitating the transfer of Li⁺ from brine into interface followed by insertion into voids. Importantly, the intrinsic oxygen vacancies derived from Zn-doping depressed the diffusion energy barrier of Li⁺, which accelerated the diffusion process of Li⁺ in the internal bulk of LiZnAl-LDH. This work provides a general strategy to overcome the existing limitations of Li⁺ recovery and deepens the understanding of Li⁺ extraction on LiAl-LDH.

锂铝层状双氢氧化物（LiAl-LDH）已成功应用于商业规模的从盐湖卤水中提取锂，然而，其应用的进一步发展受到Li+吸附性能欠佳和提取工艺不明确的阻碍。在此，开发了一种掺杂工程策略来制造新型Zn ²⁺掺杂的LiAl-LDH（LiZnAl-LDH），其具有显着更高的Li ⁺吸附容量（13.4 mg/g）和选择性（Li 的分离因子为213、834、171）⁺ /K ⁺、Li ⁺ /Na ⁺、Li ⁺ /Mg ²⁺分别），以及与原始 LiAl-LDH 相比，在罗布泊盐水中的无损可重复使用性。此外，结合实验和模拟计算发现，LiZnAl-LDH的比表面积、亲水性和对Li ⁺的表面吸引力显着提高，降低了吸附能（E _ad）和吉布斯自由能（ΔG），从而促进Li ⁺从盐水转移到界面，然后插入空隙中。^{重要的是，Zn掺杂产生的本征氧空位降低了Li +}的扩散能垒，从而加速了Li ⁺的扩散过程在 LiZnAl-LDH 的内部块中。^{这项工作提供了克服Li +}回收现有局限性的总体策略，并加深了对LiAl-LDH上Li ⁺提取的理解。