Cost-effective and efficient lithium extraction technology is vital to foster the growth of lithium industry. This paper proposed a novel approach for the high value utilization of spent LiFePO₄ (S-LiFePO₄) in the field of lithium extraction from salt lakes was proposed using spent LiFePO₄ (S-LiFePO₄) as raw material. The anode, made from spent LiFePO₄, is prepared via a sintering process, while FePO₄, obtained through chemical oxidation, is used as the cathode. Compared with commercial LiFePO₄, this system not only reduces the cost but also greatly shortens the preparation time of FePO₄ (only about 10min is required). And the electrochemical extraction system had a favorable lithium extraction capacity (29.25 mg/g) from actual brine, reducing the Mg/Li ratio from 61.4 to 0.8. This study not only achieved the low-cost preparation of electrode materials and facilitated the large-scale implementation of this process, but also proposed a high-value comprehensive utilization strategy for lithium-ion batteries recycling.

Thick electrodes greatly enhance lithium extraction capacity. However, with the increase of active substances loading, the traditional thick electrodes are more hydrophobic, severely limiting the utilization of active substances. Hence, a sulfonation process to functionalize thick electrodes was applied to enhance their wettability (~45 mg·cm⁻¹) in brine. Experimental and theoretical results show that the lithium extraction capacity of thick electrodes can be significantly improved by enhancing the electrodes hydrophilicity. At 0.8 V, the S-PVDF electrode's capacity for lithium extraction in simulated brine (41.72 mg·g⁻¹) significantly surpassed the PVDF electrode (35.72 mg·g⁻¹), and it also performed well in actual brine (28.8 mg·g⁻¹). The Mg²⁺/Li⁺ ratio in actual brine dropped from 65 to 0.37, achieving effective magnesia‑lithium separation. This method offers a novel approach to developing high-efficiency lithium extraction thick electrodes.

Improving the kinetic performance of thick electrodes is key to enhancing lithium extraction from salt lakes. Nano-melamine foam (MF), known for its unique porous structure, is ideal for building a three-dimensional (3D) conductive network, thereby boosting electrode kinetics. In our study, we developed a thick electrode (20 mg·g−1) with a 3D-conductive network by in-situ growing LiFePO4 (LFP) onto a nanoscale MF substrate. This electrode exhibited superior kinetic performance and a high lithium adsorption capacity in brine, achieving up to 32.8 mg·g−1 in just 10 min. Remarkably, even in simulated brine with a high Mg2+/Li+ ratio, it maintained an average coulomb efficiency of 62 %, significantly lowering the Mg2+/Li+ ratio from 65.6 to 0.47. It also showed exceptional stability in actual brine, maintaining an average coulomb efficiency of about 56.6 %. Our development of this high conductivity, thick electrode provides new insights into efficient lithium extraction methods.

Constructing thick electrodes with high Li+ adsorption capacity and excellent kinetic performance effectively addresses the low efficiency of lithium extraction from salt lake brines. However, an increase in the content of active material can hinder the Li+ mass transfer within the electrode, resulting in polarization and reduced kinetic performance, which ultimately affects the extraction efficiency. This study synthesized a three-dimensional(3D) conductive network-incorporated thick electrode (∼20 mg/cm2) composed of the redox graphene oxide-loaded LFP(LFP/rGO) composite through an in situ hydrothermal method. The electrode material showed excellent kinetic performance and a high adsorption capacity for Li+ in salt lake brine. Under a constant voltage of 0.8 V in Li+ solution, the Li+ adsorption capacity reached 36.78 mg·g−1 within 10 min, exhibiting an average coulombic efficiency of over 83.53 %. Furthermore, the LFP/rGO composite thick electrode exhibited a Li+ adsorption capacity of 32.82 mg·g−1, along with an average coulombic efficiency of 74.6 %, even in the West Taijinar old brine solution. Additionally, the electrode material demonstrated remarkable cycling stability, maintaining a capacity of 172.09 mAh·g−1 after 50 cycles at a 0.2C rate in a high-concentration salt lake brine. Our preparation strategy offers novel insights for high-performance lithium extraction electrodes.

Enhancing the kinetic performance of thick electrodes is essential for improving the efficiency of lithium extraction processes. Biochar, known for its affordability and unique three-dimensional (3D) structure, is utilized across various applications. In this study, we developed a biochar-based, 3D-conductive network thick electrode (∼20 mg cm−2) by in-situ deposition of LiFePO4 (LFP) onto watermelon peel biomass (WB). Utilizing Density Functional Theory (DFT) calculations complemented by experimental data, we confirmed that this The thick electrode exhibits outstanding kinetic properties and a high capacity for lithium intercalation in brines, even in environments where the Magnesia-lithium ratios are significantly high. The electrode showed an impressive intercalation capacity of 30.67 mg g−1 within 10 min in a pure lithium solution. It also maintained high intercalation performance (31.17 mg g−1) in simulated brines with high Magnesia-lithium ratios. Moreover, in actual brine, it demonstrated a significant extraction capacity (23.87 mg g−1), effectively lowering the Magnesia-lithium ratio from 65 to 0.50. This breakthrough in high-conductivity thick electrode design offers new perspectives for lithium extraction technologies.

Despite the high energy density of lithium-rich manganese-based (LR) cathode materials, the practical implementation in batteries has been impeded by the intrinsic issues regarding cycling. Herein, a coherent interface modification strategy is proposed. The LR materials are coated with a lattice-matched Li3BO3 (LBO) layer at the interface. The coating applied to the electrode has two impacts. (1) It reduces interfacial side reactions between the electrode materials and electrolyte, thereby improving structural stability. (2) It mitigates stress between solid particles, which enhances the cycling stability (83% after 500 cycles at 2C) of LR. Furthermore, the LBO coating promotes the development of a spinel-like structure on the electrode materials surface, eliminating unstable oxygen, increasing oxygen vacancy (Ov), consequently enhancing the initial Coulombic efficiency (ICE, 92.18%), and alleviating particle breakage (Young’s moduli of LR@S@LBO is 3.26 ± 1.6 GPa) after optimization. Theoretical calculations show that Ov and spinel can improve the diffusion of Li+ and the structural stability of LR materials. This work shows great potential for the rational design of high-energy-density electrode materials.