Efficient Low-Temperature Direct Lithium Extraction from Chloride Brines Enabled by High-Capacity Sorbent

Abstract

The demand for lithium, a key component in rechargeable batteries for electric vehicles and renewable energy storage systems, has surged in recent years. Meeting this demand requires efficient extraction methods that are both environmentally friendly and economically viable. This study investigates the utilization of the high-capacity sorbent amorphous aluminum hydroxide for enabling efficient direct lithium extraction at low temperatures. Traditional extraction methods often involve acid-leaching and energy-intensive processes that are not only expensive but also environmentally taxing. In contrast, our approach leverages the exceptional sorption properties of amorphous aluminum hydroxide to facilitate lithium extraction directly from brine, achieving extraction efficiencies of 94.4% in case 1 and 96.2% in case 2 at low temperatures. Kinetic modeling using the Avrami–Erofe’ev framework reveals a nucleation-growth mechanism (n = 0.71, k = 0.131 h^–1), providing quantitative insights into the solid-state phase transformation process. This method significantly reduces energy consumption and minimizes the environmental footprint. Through systematic experimentation and optimization, we demonstrate the effectiveness and scalability of our approach, highlighting its potential to revolutionize lithium extraction processes. Our findings highlight the potential of high-capacity sorbents, particularly amorphous aluminum hydroxide toward sustainable lithium production, contributing to the advancement of clean-energy technologies.

Introduction

Lithium is considered as a critical element for energy storage, electronics, and emerging clean-energy technologies, and its demand continues to rise with the global expansion of electric vehicles and stationary energy systems. , This rapid growth has intensified concerns about supply security, environmental sustainability, and the efficiency of current extraction technologies. − Conventional lithium production such as evaporation ponds, mineral processing, and solvent extraction suffers from long residence times, high water and energy consumption, and environmental burdens associated with large land footprints and chemical usage. − These limitations underscore the urgent need for more sustainable and economically viable extraction methods. Recent advances in electrochemical lithium extraction highlight the importance of materials design and ion-selective mechanisms in improving extraction performance. − Strategies such as morphology-controlled FePO₄, LMO@COF composites for high-temperature brines, and pulsed electric-field-enhanced LMO/MXene electrodes have demonstrated improved selectivity, kinetics, and stability, illustrating the potential of engineered materials for next-generation lithium recovery. −

Direct lithium extraction (DLE) technologies have therefore emerged as promising alternatives to traditional processes due to their potential for high selectivity, lower chemical consumption, and reduced environmental impact. − Among various DLE approaches, sorbent-based systems are particularly attractive because they enable selective lithium uptake from complex brines. However, conventional sorbents often suffer from high cost, structural instability, slow kinetics, or poor selectivity in the presence of competing ions such as Na⁺ and Mg²⁺. −

Layered double hydroxides (LDHs) and aluminum hydroxide-based sorbents have recently gained attention due to their tunable structure, chemical versatility, and high sorption capacities. ,− Sorption-based lithium recovery is advantageous because it minimizes energy input and supports circular economy practices by enabling lithium capture from a variety of aqueous resources. − While much research has focused on Mg²⁺/Li⁺ separation due to similar ionic radii, the equally challenging Na⁺/Li⁺ separation critical for high-salinity chloride brines remains less explored. In real brines, where sodium concentrations can exceed lithium concentrations by several orders of magnitude, developing sorbents capable of selective monovalent ion separation is essential.

Building on our previous calorimetric studies that identified thermodynamically favorable LDH compositions and the highly reactive amorphous aluminum hydroxide polytype for lithium sorption, ,− ,− the present work investigates low-temperature DLE using amorphous aluminum hydroxide as a high-capacity lithium-selective sorbent. We first examine the lithium uptake from simple chloride brines and subsequently extend the process to multi-ion brines containing Na⁺ and K⁺ to simulate realistic extraction conditions. Kinetic experiments, delithiation steps to recover LiCl, and regeneration of the sorbent via controlled reprecipitation are employed to evaluate cyclic stability and overall process feasibility. This integrated approach provides a mechanistic understanding and demonstrates a low-energy, environmentally compatible pathway for sustainable lithium production.

Experimental Section

The sorbent used for this study is amorphous Al­(OH)₃ (A-Al­(OH)₃). A-Al­(OH)₃, LiCl, NaCl, and KCl were procured from Sigma-Aldrich. All of the aforementioned chemicals were used without further purification. In case 1, the first brine simulant was prepared using LiCl, while in case 2, the second brine simulant was prepared using a mixture of LiCl, NaCl, and KCl. The pH and lithium concentrations of the first brine were 5.75 and 2220 ppm, respectively. The second brine contained 468 ppm of lithium, 4810 ppm of sodium, and 4470 ppm of potassium, respectively. Both brines represent typical concentrations found for different feedstocks such as clay mineral leachates and produced waters. pH measurements were made using an Oakton pH 700 Benchtop meter with the probe electrode calibrated against standard buffer solutions.

Lithiation

To maximize the lithium uptake in case 1, twice the stoichiometric amount of A-Al­(OH)₃ was used to form A-LDH in the lithiation process. 2.0 g of A-Al­(OH)₃, along with 20 mL of 2220 ppm Li brine solution, was placed in a screw-capped bottle (for room temperature (RT), 40 and 60 °C) or a round-bottom flask with the reflux condenser attached to a chiller (for 80 and 95 °C). The mixture was stirred continuously at various temperatures for up to 18 h. The pH was measured both before and after the lithiation process. Following centrifugation of the precipitate, the supernatant solution was decanted, and the solid was dried in an oven at 60 °C. The solid will be referred to as A-Cl-LDH corresponding to the chloride form of LDH synthesized using A-Al­(OH)₃. Similarly, in case 2, 5 g of A-Al­(OH)₃ mixed with 50 mL of brine containing mixture of LiCl, NaCl, and KCl was placed in screw-capped bottle and treated at 40 °C for 18 h, which was the optimized condition for the maximum uptake of Li.

Kinectic Studies

Kinetic experiments were conducted to study the reactivity of A-Al­(OH)₃ when it was reacted with the brine solution containing 2220 ppm of Li⁺. These experiments followed the same procedure as the lithiation process. 2 g of amorphous was added to 20 mL of Li brine solution, and the mixture was continuously stirred at 40 °C in a screw-capped bottle for 1–18 h. Following centrifugation of the precipitate, the supernatant solution was decanted, and the solid was dried in an oven at 60 °C.

Delithiation

0.25 g of A-Cl-LDH material was added to 25 mL of distilled water in a reflux condenser with continuous stirring at 95 °C for 2–10 h, as described elsewhere. , Following centrifugation of the precipitate, the supernatant solution was decanted, and the solid was dried in an oven at 60 °C.

Powder X-ray Diffractometry (PXRD)

The phase confirmation for all of the solid samples in both the lithiation and delithiation experiments was carried out by PXRD using an Empyrean X-ray diffractometer from Pan Analytical that was equipped with a Cu Kα source (2.54 Å) run at 45 kV and 40 mA and filtered with a Ni beta filter. Data were recorded in the 2θ range of 5–90° at a continuous scan rate of 4° min^–1 and with a step size of 0.02°.

Thermogravimetry (TG)

The measurements were performed on a Q-50-1665 TA analyzer (TA Instruments) to measure the water content in the LDHs. A-Cl-LDH pellets weighing about 30 mg were placed into a Pt crucible and heated from 25 to 800 °C at 10 °C/min in flowing nitrogen gas. All LDHs and Li salts were stored in a glovebox to avoid any adsorption of water.

Inductively Coupled Plasma-Optical Emission Spectrometry (ICP-OES)

Metal content of aqueous solutions was measured by ICP-OES analysis using an iCAP 7400 spectrometer (Thermofisher Scientific) equipped with a prepFast M5X automatic dilution sample loader (Elemental Scientific, Omaha, Nebraska). Mobile phase and diluent were 2% ultrapure nitric acid in distilled water, purified with a Milli-Q purification system (Millipore). Internal standard was 5 ppm yttrium procured from RICCA. Commercial elemental standards for lithium and aluminum procured from Millipore Sigma-Aldrich were used to generate 7-point standard curves. Limit of detection was 0.5 ppm, according to the manufacturer. To prepare the samples, they were dissolved in Optima grade 8 M nitric acid (HNO₃, Sigma-Aldrich). The samples are diluted at least 10-fold with 2% nitric acid in H₂O. To determine the measurement uncertainty, an expanded uncertainty approach was used, considering components such as measurement uncertainty, calibration uncertainty, and quality control uncertainty (% relative difference).

Brunauer–Emmett–Teller

The Brunauer–Emmett–Teller surface area, Barrett–Joyner–Halenda (BJH) cumulative mesopore volume, and t-plot pore volume were evaluated from N₂ adsorption isotherms at 77 K obtained with Micromeritics Tristar 3000 and MicroActive V6 analyzers. The samples were degassed at 120 °C for 15 h prior to measurements.

Results and Discussion

Case 1: the impact of temperature on the lithium uptake from the simple Li solution by A-Al­(OH)₃ is evaluated, as shown in Table , Figure . The theoretical lithium loading capacity per gram of the sorbent is calculated to be 6.41 mequiv/g. At RT, the lithium uptake was 30.3%, with a loading of 6.72 mg/g (0.97 mequiv/g), which contributes to 15% theoretical capacity. As the temperature increases to 40 °C, the uptake dramatically increased to 94.4%, achieving 20.96 mg/g (3.02 mequiv/g) loading which contributes to 47% theoretical capacity. Further increasing the temperature to the range of 60 to 95 °C showed similar lithium uptake percentages of 98.4%, 96.1%, and 92.7%, respectively, with corresponding loadings and theoretical capacity between 46 and 49% (Figure ). These results indicate that increasing the temperature significantly enhances the lithium uptake and loading, with the highest uptake observed at 60 °C. Beyond 40 °C, there was no major difference in the percentage uptake of lithium or loading. Therefore, the 40 °C synthesis was chosen for further experiments due to its lower energy requirements and more moderate temperatures. In the previous study on sulfate brine, similar experiments achieved a lithium loading of 1.74 mequiv/g, which is relatively lower than the lithium loading observed in the chloride brine studies conducted in this work.

1. Lithium Uptake Percentage and Loading by A-Al­(OH)₃ at Different Temperatures for 18 h in 2220 ppm LiCl Brine.

temperature	pH before contact	pH after uptake	concentration of Li in the decant (μg/mL)	% uptake	loading (mg Li/g)	loading (meq Li/g)
RT	7.60	6.45	1547.325	30.27	6.72	0.97
40 °C	7.62	4.80	123.227	94.44	20.96	3.02
60 °C	7.70	4.58	34.753	98.43	21.84	3.15
80 °C	7.68	4.99	86.414	96.10	21.33	3.07
95 °C	7.73	5.09	162.83	92.66	20.56	2.96

^a±5% uncertainty.

1.

Temperature vs lithium uptake in a single lithiation step.

It is important to consider that the uptake reported in Table reflects loading vs capacity. The latter would be expected to be twice the loading measured in that the stoichiometric amount of A-Al­(OH)₃ used in the experiment was twice what is required to achieve the ideal A-LDH stoichiometry LiCl·Al₂(OH)₆·xH₂O. Moreover, capacity would properly be the maximum level of loading that would be achieved for the sorbent in equilibrium with the feed solution at its initial Li concentration. Capacity thus would reflect the loading of the material in a column, for example, driven to full breakthrough. In batch tests, it would be obtainable by successive contacts of the loaded sorbent with fresh solution until no more Li is sorbed, which was not done here.

The dried loaded solids isolated from the sorption of Li from the simple Li solution by A-Al­(OH)₃ were subjected to analysis upon dissolution in nitric acid. Table presents the ICP-OES results, showing the lithium content in the solid sorbents at various temperatures. At RT, the lithium content is 1.19 mequiv/g. When the temperature is increased to 40 °C, the lithium loading significantly rises to 3.12 mequiv/g. Notably, this loading remains consistent at 60 °C with 3.12 mequiv/g and shows only slight variation at higher temperatures, with 2.90 mequiv/g at 80 °C and 2.62 mequiv/g at 95 °C. These data indicate that the lithium loading in the solid sorbent stabilizes at 40 °C, and further temperature increases do not lead to substantial improvements. Consequently, 40 °C is considered optimal for achieving high lithium loading with balanced energy requirements.

2. ICP-OES Results of the Solids Depicting Amount of Li with Varying Temperatures.

Temp.	Al (μg/g)	Li (μg/g)	(mg Li/g sorbent)	(meq Li/g sorbent)
RT	251742.5	6003.385	8.25	1.19
40 °C	235813.3	14755.33	21.64	3.12
60 °C	245139.6	15358.18	21.67	3.12
80 °C	258775.7	15043.26	20.11	2.90
95 °C	267307.6	14056.40	18.19	2.62

^a±5% uncertainty.

Inferred lithium loadings shown in column 5 of Table are comparable to those in column 7 of Table that were determined directly from the uptake data. The resulting estimated loading values match reasonably well with those shown in Table . Thus, mass balance is consistent with formation of the LDH having the stoichiometry LiCl·Al₂(OH)₆·3H₂O that we documented previously. The PXRD patterns of the A-Cl-LDHs formed at different temperatures are shown in Figure . At RT, the presence of a bayerite phase is observed, along with the LDH phase. In contrast, the PXRD patterns for the A-Cl-LDHs formed at temperatures ranging from 40 to 95 °C display a single phase corresponding to chloride LDH. This indicates that higher temperatures favor the formation of a pure LDH phase without impurities.

2.

PXRD pattern showing A-Cl-LDHs at different temperatures.

The lithiation process was investigated through kinetic experiments with the results summarized in Table . At 40 °C, the lithium uptake increased progressively over time, as reflected in the decreasing concentration of lithium in the decant and the corresponding increase in loading. After 1 h, the lithium uptake was 20.47%, with a loading of 4.54 mg/g (0.65 mequiv/g). This uptake increased to 47.88% after 2 h, with a loading of 10.62 mg/g (1.53 mequiv/g). A notable increase was observed after 4 h, with 60.45% uptake and a loading of 13.41 mg/g (1.93 mequiv/g). The lithium uptake continued to rise gradually, reaching 75.27% after 10 h (loading of 16.70 mg/g, 2.40 mequiv/g) and 85.76% after 16 h (loading of 19.03 mg/g, 2.74 mequiv/g). The highest uptake was observed after 18 h, with 94.45% and a loading of 20.96 mg/g (3.02 mequiv/g). These results indicate a clear correlation between the reaction time and lithium uptake, with significant improvements observed up to 18 h (Figure ). The ICP results of the solids obtained with varying time for the lithiation process are shown in Table S1.

3. Illustrating the Li Loading and Uptake Percentage at 40 °C across Varying Times.

time (h)	concentration of Li in the decant (μg/mL)	% uptake	loading (mg/g)	loading (meq/g)
1	1764.838	20.47	4.54	0.65
2	1156.531	47.88	10.62	1.53
4	877.569	60.45	13.41	1.93
6	818.299	63.12	14.01	2.02
8	831.860	62.51	13.87	1.99
10	548.809	75.27	16.70	2.40
12	551.947	75.13	16.67	2.40
14	586.899	73.55	16.32	2.35
16	316.051	85.76	19.03	2.74
18	123.227	94.45	20.96	3.02

^a±5% uncertainty.

3.

Kinetic profile of the lithium uptake by amorphous Al­(OH)₃ at 40 °C.

Kinetic analysis at 40 °C (Figure , Table ) reveals lithium uptake reaches 94.4% after 18 h. Following the Avrami–Erofe’ev framework established by Fogg & O’Hare for LiCl-gibbsite transformations, we fitted a nucleation–growth model yielding k = 0.131 h^–1 and n = 0.71 ± 0.14. The excellent fit (R ² = 0.969) and Avrami exponent are consistent with instantaneous nucleation followed by two-dimensional diffusion-controlled growth, consistent with the irreversible topotactic phase transformation confirmed by XRD. Full details of the Avrami–Erofe’ev kinetic fitting, including nomenclature, fitted parameters, goodness-of-fit statistics, and residual analysis, are provided in Tables S6–S8.

Kinetic experiments were conducted to evaluate the delithiation process, specifically focusing on the amount of lithium that leached out of the LDH structure over time. The results, plotted in Figure and presented in Table S2, show a substantial increase in lithium release within the first 3 h, reaching an apparent maximum of 70.1% lithium release. Beyond this initial period, the lithium release rate stabilizes with only minor fluctuations observed. This plateau behavior implies that the majority of lithium is released within the initial few hours and extending the delithiation time beyond this period does not enhance the release. Figure demonstrates the impact of time on lithium release, highlighting the efficiency of the process at elevated temperatures. These findings suggest that the delithiation kinetics are rapid initially but plateau as the system approaches equilibrium, highlighting the efficiency of the process within the first few hours.

4.

Li release vs time in the delithiation step at 95 °C.

The ICP results of the solids obtained at various times during the delithiation process are presented in Table S3. The data indicate that the percentage of lithium remaining in the solid decreases significantly within the first few hours, correlating with the increased lithium release observed in the solution phase. Figure illustrates the formation of the bayerite phase during delithiation, confirming the structural transformation of the sorbent material. Additionally, delithiation was conducted in a single cycle, achieving substantial lithium recovery from the loaded material. However, by incorporating an additional cycle, the lithium extraction efficiency can be increased to approximately 95%. This suggests that multiple stages of delithiation could be a viable strategy for enhancing the recovery of lithium from the sorbent material, thereby improving the overall efficiency of the extraction process.

5.

(a) PXRD patterns and (b) FTIR spectra for Sigma-Aldrich, bayerite, and regenerated Al­(OH)₃.

The SEM images presented in Figure S2 clearly demonstrate that the crystal size of gibbsite is larger than that of bayerite, while the amorphous phase exhibits no defined crystalline structure. This observation is consistent with the pore structure and BET surface area data presented in Table , which show that amorphous aluminum hydroxide (A-Al­(OH)₃) possesses a significantly larger pore volume and surface area compared to the crystalline polymorphs, bayerite, and gibbsite. These results confirm the expected inverse relationship between crystal size and surface area, further validating the distinct structural and textural characteristics of the three aluminum hydroxide phases. Previous stability measurements, combined with surface area and pore structure analysis, confirm that A-Al­(OH)₃ is the most effective sorbent for lithium extraction among the tested materials. This superior performance is attributed to its enhanced pore characteristics, providing more active sites for lithium adsorption, and its inherent high reactivity, making it highly suitable for large-scale lithium extraction operations.

4. Pore Structure Characterization and BET Surface Area of Al­(OH)₃ .

sample	mesopore volume (cm3/g)	BET surface area (m2/g)
A-Al(OH)3	0.131	48.12
B-Al(OH)3	0.0533961	14.54
G-Al(OH)3	0.00853974	3.67

^aA: Amorphous, B: Bayerite, G: Gibbsite.

Kinetic experiments for lithiation were conducted to determine if A-Al­(OH)₃ exhibited similar reactivity and performance in the presence of a chloride brine, as observed with a sulfate brine in a previous study. However, in the case of the chloride brine, the maximum uptake of Li⁺ required 18 h, compared to only 3 h for the sulfate brine. This difference is attributed to the divalent anion SO₄ ^2– being a stronger hydrogen bonder than the monovalent Cl^– anion. The weaker hydrogen bonding of Cl^– requires more time to react with the sorbent material to uptake Li⁺. The same reasoning applies to delithiation: the weak hydrogen-bonding Cl^– anion requires less time (3 h) to leach out Li as LiCl, whereas the sulfate required 24 h over 4 cycles/steps to leach out Li as Li₂SO₄. , In conclusion, using the sulfate brine, lithiation is faster, but delithiation is slower and requires additional steps, whereas with the chloride brine, lithiation takes longer but delithiation is faster.

The experiments revealed that lithiation can be effectively achieved at temperatures as low as 40 °C, a significant improvement over previously required higher temperatures and hydrothermal conditions. ,, This study demonstrates the selective direct extraction of Li⁺ ions using A-Al­(OH)₃ through a liquid–solid lithiation reaction followed by an acid-free delithiation process. The lithiation process achieved an efficiency of approximately 95% and a lithium sorption loading of around 21.0 mg/g. The sorbent exhibited high selectivity during lithiation, and nearly 70% recoverability of lithium from the sorbent material was observed during delithiation. Notably, substantial recovery of the sorbent was achieved by employing a second cycle of delithiation, see Table S4. PXRD pattern had no traces on A-Cl LDH peaks; see Figure S1.

Case 2: lithiation and delithiation experiments were conducted in parallel to the kinetic experiments to determine whether A-Al­(OH)₃ exhibited the selectivity of lithium over sodium and potassium. About 5 g of Al­(OH)₃ in 50 mL of brine containing mixture of LiCl, NaCl, and KCl at 40 °C for 18 h picked up ∼96.2% of lithium and less than 1% Na and K (as shown in Table ). The precipitated solids were separated by centrifugation and further washed 5 times with deionized water kept for air drying at ambient temperature. Solid A-Cl-LDH was delithiated in two steps at 95 °C for 18 h, resulting in substantial recovery of lithium. Since this work was carried out in parallel with our kinetic experiments, we used nonoptimized parameters for the delithiation. The delithiated LDH was found to have a bayerite, B-Al­(OH)₃ phase, similar to the results observed previously. To regenerate the sorbent and mitigate the low reactivity and performance of delithiated LDH, 2 g was dissolved in 10 mL of 8.5 M nitric acid. The pH of the solution was adjusted to 4.95 by dropwise addition of ∼10 mL of ammonium hydroxide (28% V/V). The precipitate obtained was amorphous, regenerated Al­(OH)₃. Figure shows PXRD patterns and FTIR spectra on the Sigma-Aldrich Al­(OH)₃, delithiated LDH and regenerated Al­(OH)₃, confirming the transformation of delithiated LDH to amorphous Al­(OH)₃ using the regeneration process. The XRD patterns of commercial (Sigma-Aldrich) and regenerated Al­(OH)₃ as seen in Figure a show similar features. The regenerated Al­(OH)₃ displays broad peaks at 18°, 40°, and 64° 2θ that correspond to sharp peaks in the delithiated phase. These broad peaks could suggest the presence of some crystallinity in the structure. The broad and smooth absorption bands in the ranges of 400–900 and 3200–3700 cm^–1 in Figure b correspond to the Al–O and O–H stretching vibration. The FTIR spectra for the Sigma-Aldrich Al­(OH)₃ and the regenerated Al­(OH)₃, as shown in Figure , show similar peaks validating the ability of the regeneration process. The O–H peak in the delithiated LDH phase shows a more significant shift toward higher frequency, accompanied by a decrease in intensity and higher frequency shift of the C–O stretch.

5. ICP-OES Results Illustrating Li Selectivity over Na and K for A-Al­(OH)₃ .

experiment	concentration of Li in the decant (μg/mL)	concentration of Na in the decant (μg/mL)	concentration of K in the decant (μg/mL)	% Li pick up
brine simulant	468.75	4810.375	4470.017
lithiation (5 g)	18.709	4736.375	4372.106	96

^a±5% uncertainty.

The FTIR spectral data for all Sigma-Aldrich Al­(OH)₃, delithiated LDH Al­(OH)₃, and regenerated A-Al­(OH)₃ phases are shown in Table S5. Sigma-Aldrich delithiated LDH “g” of the regenerated Al­(OH)₃ was reused as a sorbent twice using the same procedure as described above with 20 mL of the brine, and it showed a lithium pickup of 45.9%. The percentage lithium pickup is lower than that observed for virgin Al­(OH)₃, but that can be ascribed to a lower solid to liquid ratio of 0.5 g to 20 mL compared to 2 g:20 mL used above.

Conclusions

The demonstrated 96% lithium selectivity over Na⁺ and K⁺ addresses a critical challenge in DLE as many Mg/Li separation processes struggle with Li⁺/Na⁺ discrimination. For brines containing divalent cations (Mg²⁺, Ca²⁺), established preprocessing methods such as chemical precipitation or nanofiltration could remove these species prior to lithium extraction, positioning this Al­(OH)₃-based process as a complementary technology within integrated brine processing flowsheets. The acid dissolution and precipitation of the delithiated Al­(OH)₃ create a low-cost pathway for circular economy. Our results show that lithiation can be achieved efficiently at temperatures as low as 40 °C, with a lithium sorption loading reaching approximately 20.96 mg·g^–1 and an efficiency close to 95%. The sorbent displayed excellent selectivity during the lithiation process, with nearly 70% of the material recoverable during delithiation and substantial recovery achieved through a second cycle. The kinetic analysis establishes this process as a topotactic phase transformation rather than surface adsorption. The Avrami exponent (n = 0.71) indicates instantaneous nucleation, followed by two-dimensional diffusion-controlled growth, providing a mechanistic framework for rational process optimization. These findings suggest that the proposed method is not only efficient but also sustainable, making it a promising approach for large-scale DLE. Looking ahead, further research is needed to optimize the performance of high-loading sorbents, scale up the production process, and validate the economic feasibility of our approach on a commercial scale. Ensuring the scalability and cost-effectiveness of these methods will be crucial for their adoption in industrial-scale lithium extraction. The promising results from this study pave the way for future advancements in sustainable lithium extraction technologies.

The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsomega.5c11802.

• XRD plots for bayerite, delithiated LDH, and A-Cl-LDH; ICP-OES results of the solids depicting amount of Li with varying times; Li release vs time; ICP-OES results of the solids depicting amount of Li remaining after delithiation with varying times; second cycle of delithiation using the partially delithiated A-Cl LDH from the first cycle; FTIR spectral peak positions and respective assigned peaks for virgin, bayerite, and regenerated Al­(OH)₃; Avrami–Erofe’ev kinetic parameters for the lithium uptake by amorphous Al­(OH)₃ at 40 °C; experimental and Avrami–Erofe’ev fitted lithium uptake capacities for amorphous Al­(OH)₃ at 40 °C; nomenclature for Avrami–Erofe’ev kinetic analysis; SEM images of amorphous Al­(OH)₃, bayerite, and gibbsite; Avrami–Erofe’ev model; and Avrami exponent interpretation (PDF)

The authors declare no competing financial interest.