Lithium-rich manganese-based (LR) cathodes can deliver high capacity through oxygen redox, but irreversible oxygen release often causes structural degradation, voltage decay, and poor cycling stability. Herein, we propose a Fick's law–guided gradient molybdenum (Mo) doping strategy to simultaneously stabilize bulk lattice oxygen and protect surface interfaces. Gradient-distributed Mo forms strong Mo–O bonds that suppress oxygen loss, while high-valent Mo induces an in situ Li₂MoO₄ coating and a partial spinel structure, mitigating electrolyte erosion and facilitating Li⁺ diffusion. The optimized LR@S-Mo cathode delivers a reversible capacity of 195.1 mAh·g⁻¹ with 88.6% retention after 300 cycles at 1C. Theoretical calculations support that Mo doping reduces the Li⁺ diffusion barrier and enhances oxygen stability. This work provides a unified surface-to-bulk modification route for high-energy-density LR cathodes. In this work, a surface-enriched, depth-dependent Mo distribution is constructed based on a diffusion-guided design, accompanied by an in situ Li₂MoO₄/spinel surface layer, which correlates with improved electrochemical stability of lithium-rich Mn-based cathodes.

Lithium-rich manganese-based layered oxides (LR) are promising cathodes for high-energy-density lithium-ion batteries, but their practical application is hindered by severe voltage decay, capacity fading, and interfacial instability caused by oxygen release and sluggish Li⁺ diffusion. Here, we report a rapid surface engineering strategy that integrates Na⁺ doping and spinel phase formation to construct ultra-thin and uniform cathode–electrolyte interphase (CEI) films. Density functional theory calculations reveal that Na⁺ incorporation stabilizes lattice oxygen by forming strong Na-O bonds and reduces the Li⁺ diffusion barrier by 0.22 eV. Experimentally, Na⁺ doping expands the Li layer spacing and generates oxygen vacancies, which further facilitate Li⁺ transport. Consequently, the modified cathode exhibits enhanced interfacial stability and suppressed oxygen evolution, leading to a high discharge capacity of 191 mAh·g-1 with 83.6% retention after 300 cycles at 1C, and 107.8 mAh·g⁻¹ even at 10C. This scalable and cost-effective strategy offers new insights into interfacial design for the commercialization of lithium-rich cathodes.

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.

Electrochemical extraction of lithium (ELE), as a green lithium extraction technology, is of great significance to the exploitation of lithium resources in salt lakes and the sustainable development of the new energy industry. However, the low efficiency and competition of impurity ions limit its large-scale application. In this paper, the current research progress is reviewed from the viewpoint of reaction tank design, electrode material modification, reaction tank process parameter optimization and multi-technology coupling. Additionally, through in-depth research and exploration of these key issues, it is expected to improve the efficiency of electrochemical lithium extraction, reduce energy costs, and promote the practical application and popularization of lithium extraction technology in salt lakes. Finally, this paper discussed the existing challenges and outlooks to improve the performance of ELE, meeting the rising global demand for lithium sources.

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.

In response to the problems of large interfacial diffusion resistance and low lithium extraction efficiency in traditional high-loading film electrodes during lithium extraction from salt lakes by the electrochemical de-intercalation method, this paper presents an interfacial engineering strategy based on the carboxymethyl cellulose lithium (CMC[sbnd]Li) binder. By modulating the structure of the inner Helmholtz plane (IHP) of the electrical double layer and enlarging the effective specific surface area, the migration rate of Li⁺ and the lithium extraction efficiency are remarkably enhanced. In this study, a CMC-Li composite electrode sheet was prepared using Spent LiFePO₄ as the raw material. It was demonstrated that the carboxyl (-COOH) and hydroxyl (-OH) functional groups of CMC-Li can be directionally adsorbed on the electrode surface. This adsorption event reconstructs the IHP-layer structure, reduces the solvation energy barrier of Li⁺, and increases the effective specific surface area of the film electrode. As a result, the contact angle decreased from 130.01° to 55.17°. Furthermore, in the CMC-Li system, the lithium extraction rate in simulated brine increased from 0.33 mg·g⁻¹·min⁻¹ to 0.69 mg·g⁻¹·min⁻¹, while the energy consumption decreased by a factor of 3. In the West Taijinar brine, the lithium extraction capacity reached 23.01 mg·g⁻¹ with a concurrent dramatic reduction in the Mg/Li ratio from 141 to 0.42. These results indicate that the CMC-Li system exhibits excellent lithium extraction performance and high selectivity. Overall, this study proposes a groundbreaking interfacial design concept that achieves both high efficiency and sustainability for lithium extraction from salt lake brines.

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.

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.

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.