Selective Recovery Of Lithium Research Articles

Water-aerosol-assisted roasting for selective lithium extraction from spent lithium-ion batteries

Selective extraction of lithium from spent lithium-ion batteries (LIBs) represents a promising solution for efficient lithium recovery. Herein, a water-aerosol-assisted roasting technology is proposed to selectively extract lithium from spent lithium transition metal oxides (LTMOs) cathodes. In an exemplary recycling of spent LiCoO2, the cathode material undergoes a low-temperature (350°C) chlorinating roast process to convert it into metal chlorides, followed by a higher-temperature (500°C) roasting to facilitate the selective pyrolysis of CoCl2. The presence of water-aerosol significantly enhances the selective pyrolysis process of CoCl2, reducing roasting time eightfold compared to conventional air roasting. Subsequent water-leaching effectively extracts 99.1 % of lithium as LiCl, while only 0.2 % of cobalt is extracted, ensuring selective lithium recovery. The resulting high-purity LiCl solution and Co3O4 residue are directly utilizable for producing battery-grade Li2CO3 and LiCoO2, respectively. Regenerated LiCoO2 demonstrates excellent cycling stability, retaining 90.5 % of its capacity after 300 cycles at 1C rate. Moreover, this method is applicable to ternary cathodes (NCM) black mass, offering a sustainable, robust, and cost-effective approach for lithium extraction from spent LIBs.

Selective lithium recovery from waste lithium-ion batteries by H2SO4 roasting focused on process intensification and conversion mechanism

The purpose of this study is to prove the feasibility, efficiency and selectivity of lithium recovery from waste lithium-ion batteries (LIB) via sulfuric acid roasting-water leaching by thermodynamic analysis and experimental verification. The feasibility was proved by Gibbs free energy calculations and experiments. Then, the effects of H2SO4 concentration, roasting temperature and roasting time were assessed on the leaching rate of valuable metals. The results indicate that the leaching efficiency of lithium increases firstly and then decreases with the increase of H2SO4 concentration, roasting temperature and roasting time, more than 91 % lithium are leached under optimized experimental conditions: 50 wt% H2SO4, roasting temperature of 650°C, and roasting time of 2 h. Meanwhile, the selectivity of lithium is up to 88 % which means overwhelming majority lithium have been separated completely. In addition, the factors which cause sintering phenomenon such as high temperature and longtime roasting will change the microstructure of roasted product extremely, which is inconducive to the subsequent water leaching. The investigations of the phase conversion mechanism by thermodynamic simulation and instrumental characterization indicated that the leaching behaviors of valuable metals might be influenced by the different reaction pathways of the compounds while changing roasting conditions. The recovery process can be divided into two stages: the partial structure of LiNixCoyMnzO2 was destroyed to form metal sulfates at ambient temperature and the solid phase reaction between unreacted LiNixCoyMnzO2 which contained Li+ in the unstable layered structure with transition metal sulfates at high temperature. The fully reduced low-valence states are mainly (NiO)0.75(MnO)0.25 and CoO, and basically all Li within the crystalline LiNixCoyMnzO2 was de-intercalated and transformed to soluble Li2SO4. These results further confirm the advantages of H2SO4 roasting on selective Li recovery, and provide a better understanding of conversion mechanism by combining theory and experiments.

Selective recovery of lithium from used lithium-ion batteries spent via grain boundary reconstruction reaction

The demand for lithium resources on the market has increased significantly as a result of the emergence and advancement of the new energy industry. However, improper handling leads to the generation of large amounts of hazardous waste, including spent lithium batteries. The recovery of lithium from these batteries has dual importance in protecting the environment and effectively recycling secondary resources. Herein, a green process for selective extraction of lithium from discarded lithium batteries was proposed. Sodium thiosulfate mixed with waste lithium battery powder was calcined at 600 °C for 90 min, when the molar ratio of sodium thiosulfate to lithium in the raw material was 0.5, and over 99 % lithium can be selectively preferentially extracted. During the roasting process, lithium in the raw materials was converted into water-soluble LiNaSO4, and transition metal oxides after calcination existed as water-insoluble oxides or sulfides, and the goal of preferential lithium extraction can be achieved by simple immersion in water. Lithium-containing leachate was purified by cerium carbonate and NaOH. After removing a small amount of Ni, Co, Mn, Al, Ca, and F impurities, the prepared lithium carbonate had a purity greater than 99.50 %, which met the standard of battery-grade lithium carbonate. This study introduces an approach to the selective extraction of lithium from lithium-containing solid waste, which effectively simplifies the recycling separation procedure and provides support for resource utilization of lithium-containing solid waste.

High-Performance Crown Ether-Modified Membranes for Selective Lithium Recovery from High Na+ and Mg2+ Brines Using Electrodialysis

The challenge of efficiently extracting Li+ from brines with high Na+ or Mg2+ concentrations has led to extensive research on developing highly selective separation membranes for electrodialysis. Various studies have demonstrated that nanofiltration membranes or adsorbents modified with crown ethers (CEs) such as 2-OH-12-crown-4-ether (12CE), 2-OH-18-crown-6-ether (18CE), and 2-OH-15-crown-5-ether (15CE) show selectivity for Li+ in brines. This study aims to develop high-performance cation exchange membranes (CEMs) using CEs to enhance Li+ selectivity and to compare the performance of various CE-modified membranes for selective electrodialysis. The novel CEM (CR671) was modified with 12CE, 18CE, and 15CE to identify the optimal CE for efficient Li+ recovery during brine electrodialysis. The modification process included polydopamine (PDA) treatment and the deposition of polyethyleneimine (PEI) complexes with the different CEs via hydrogen bonding. Interfacial polymerization with 1,3,5-benzenetricarbonyl trichloride-crosslinked PEI was used to create specific channels for Li+ transport within the modified membranes (12CE/CR671, 15CE/CR671, and 18CE/CR671). The successful application of CE coatings and Li+ selectivity of the modified membranes were verified through Fourier-transform infrared spectroscopy, zeta-potential measurements, and electrochemical impedance spectroscopy. Bench-scale electrodialysis tests showed significant improvements in permselectivity and Li+ flux for all three modified membranes. In brines with high Na+ and Mg2+ concentrations, the 15CE/CR671 membrane demonstrated more significant improvements in permselectivity compared to the 12CE/CR671 (3.3-fold and 1.7-fold) and the 18CE/CR671 (2.4-fold and 2.6-fold) membranes at current densities of 2.3 mA/cm2 and 2.2 mA/cm2, respectively. At higher current densities of 14.7 mA/cm2 in Mg2+-rich brine and 15.9 mA/cm2 in Na+-rich brine, the 15CE/CR671 membrane showed greater improvements in Li+ flux, approximately 2.1-fold and 2.3-fold, and 3.2-fold and 3.4-fold compared to the 12CE/CR671 and 18CE/CR671 membranes. This study underscores the superior performance of 15CE-modified membranes for efficient Li+ recovery with low energy demand and offers valuable insights for advancing electrodialysis processes in challenging brine environments.

Ion-Exchange Membranes Extract Lithium From North Sea Oilfield Brines

_ This article, written by JPT Technology Editor Chris Carpenter, contains highlights of paper SPE 215585, “Lithium Extraction From North Sea Oilfield Brines Using Ion-Exchange Membranes,” by Botelho Disu, Roozbeh Rafati, and Amin S. Haddad, University of Aberdeen, et al. The paper has not been peer reviewed. _ The annual demand for lithium for low-carbon technology applications has been growing exponentially. A necessity exists in the current environment for continuous lithium production from both conventional sources and novel extraction sites from alternative brine resources such as oil fields and geothermal sites. in the complete paper, the lithium potentiality of the UK North Sea is evaluated. Identification of North Sea Lithium-Rich Oil and Gas Fields Maps show lithium-ion concentration diffusing from 55 ppm in the western region into low concentrations in the central, northern, and eastern regions of the UK North Sea. Such estimates suggest lithium enrichment in oilfield brine from the Beatrice, Clymore, Gannet, Cly, Auk, and Flumar fields. However, because such map distribution of lithium is achieved based only on one-third of the imputed data, a correlative evaluation with the entire body of data is needed to provide a much more feasible interpretation. When lithium distribution was evaluated simultaneously with strontium/iron/potassium (Sr/Fe/K) total dissolved solids, the rich brine was primarily located across the central, eastern, southern, and western fields. The central and eastern concentrations were estimated to have a lithium-rich brine with concentrations of up to 40 ppm, with lithium-ion presence gradually increasing toward the east. Most of the fields in this region are oil fields, including Montrose, Arbroath, Ula, Nelson, Brisling, Gyda, Ekofisk, and Bream, with Harald possibly being the only gas field with lithium-enriched brine. On the other hand, the lithium-rich fields in the southern and western regions are all gas fields, including the Esmond, Anglia, Lemman, Ann, and Viking fields. Statement of Theory and Definition The economic feasibility of lithium extraction from brine has been observed to be a function of its initial concentration. For oilfield brines, when using novel direct-lithium-extraction (DLE) technologies, the brine concentration economic feasibility for production is reduced to a cutoff benchmark of 50 ppm. However, ongoing developments in DLE technologies envision a feasible, efficient, and highly selective recovery of lithium from brines with low concentrations, even sea water. Manganese ion-sieve powder is a DLE technology that has gathered growing interest. However, one of the main challenges of its application in continuous industrial processes consists of operational challenges that its original powder form can cause. Therefore, forming is necessary if ion-sieve adsorbents are to have an industrial application. This paper has reported and discussed the experimental results of forming the adsorbent powders into different ion-exchange membranes (foam, flat sheet, and granular spherical beads) and their application for lithium extraction from simulated North Sea brine. The complete paper details the description and application of experimental equipment and processes.

Selective lithium recovery from lithium precipitation mother liquor by using a diketone-based solvent

Lithium recovery from lithium precipitation mother liquor is an important point for improving lithium resource utilization efficiency. In this study, a modified β-diketone based organic solvent was developed. DBM was selected as extractant, which has the advantage of low cost compared to fluor-diketones. Organic phosphate TBP was used instead of traditional alkylphosphine oxide as co-extractant. The results show that TBP has the ability to inhabit the extraction of sodium so that it is positive for separation factor of lithium to sodium. Simultaneously, TBP plays the role of diluent, thus improving two-phase separation performance significantly. The phase separation time is only tens of seconds, which is much less than that of alkylphosphine oxide co-extraction system. Besides, low cost and low viscosity properties of TBP avoid the limitation of additive amount, which means that it has the industrial feasibility to improve the extraction performance by increasing TBP concentration. The developed extraction solvent has the combination sequence of H+ > > Li+ > > Na+. By using optimized solvent of 0.4 mol/L DBM and 1.2 mol/L TBP dissolved in sulfonated kerosene, single-stage lithium extraction rate is 99.96 % and separation factor of lithium to sodium reaches >160,000 at the O/A phase ratio of 1:1.

Selective lithium recovery from pyrolyzed black mass through optimized caustic leaching

This study presents a new method for selectively extracting lithium (Li) from pyrolyzed lithium-ion batteries (LIBs) black mass (BM) using a novel caustic (NaOH) leaching process. The efficiency of the NaOH leaching has been evaluated by response surface methodology (RSM), and the effects of leaching parameters on Li leaching efficiency (LE) and selectivity have been discussed in terms of leaching mechanism based on thermodynamics and kinetics studies. The results show that caustic leaching has excellent selectivity towards Li with no detectable leaching for nickel (Ni), manganese (Mn), cobalt (Co), and copper (Cu), LE up to ∼81 % Li. However, caustic leaching coextracts aluminium with Li. Further, Li is recovered from leach solution as lithium hydroxide (LiOH) using evaporative crystallization or lithium carbonate (Li2CO3) with Na2CO3 addition and CO2 injection. Li2CO3 recovered via CO2 injection has the highest purity at ∼93 %, surpassing the Li2CO3 purity levels obtained through precipitation with Na2CO3 (∼82 %) and LiOH (∼21 %) retrieved via evaporative crystallization.

Improved recovery of lithium from spent lithium-ion batteries by reduction roasting and NaHCO3 leaching

Lithium supply risk is increasing and driving rapid progress in lithium recovery schemes from spent lithium-ion batteries (LIBs). In this study, a facile recycling process consisting mainly of reduction roasting and NaHCO3 leaching was adopted to improve lithium recovery. The Li of spent LiNixCoyMn1−x−yO2 powder were converted to Li2CO3 and LiAlO2 with the reduction effect of C and residual Al in the roasting process. NaHCO3 leaching was utilized to selectively dissolve lithium from Li2CO3 and water-insoluble LiAlO2. The activation energy of NaHCO3 leaching was 9.31 kJ∙mol−1 and the leaching of lithium was a diffusion control reaction. More than 95.19 % lithium was leached and recovered as a Li2CO3 product with a purity of 99.80 %. Thus, this approach provides a green path to selective recovery of lithium with good economics.

Selective lithium recovery and regeneration of ternary cathode from spent lithium-ion batteries: Mixed HCl-H2SO4 leaching-spray pyrolysis approach

The recycling of spent lithium-ion batteries (LIBs) is crucial for environmental protection and resource sustainability. However, the economic recovery of spent LIBs remains challenging due to low Li recovery efficiency and the need for multiple separation operations. Here, we propose a process involving mixed HCl-H2SO4 leaching-spray pyrolysis for recycling spent ternary LIBs, achieving both selective Li recovery and the preparation of a ternary oxide precursor. Specifically, the process transforms spent ternary cathode (LiNixCoyMnzO2, NCM) powder into Li2SO4 solution and ternary oxide, which can be directly used for synthesizing battery-grade Li2CO3 and NCM cathode, respectively. Notably, SO42− selectively precipitates with Li+ to form thermostable Li2SO4 during the spray pyrolysis, which substantially improves the Li recovery efficiency by inhibiting Li evaporation and intercalation. Besides, SO2 emissions are avoided by controlling the molar ratio of Li+/SO42− (≥2:1). The mechanism of the preferential formation of Li2SO4 is interpreted from its reverse solubility variation with temperature. During the recycling of spent NCM811, 92% of Li is selectively recovered, and the regenerated NCM811 exhibits excellent cycling stability with a capacity retention of 81.7% after 300 cycles at 1 C. This work offers a simple and robust process for the recycling of spent NCM cathodes.

Selective Extraction of Lithium from Spent-NMC Battery Cathodes Using Sodium Hydroxide as a Leaching Agent at Elevated Temperatures

Introduction: The demand for lithium-ion batteries (LIBs) is rapidly increasing due to the growth of the electronics and electric vehicle industries. Even though the batteries are rechargeable, their storage capacity decreases, and they eventually end up being wasted. Recycling the spent LIBs is necessary to reduce the environmental impact and utilize the precious metals contained in the waste Methods: The present work focuses on the selective recovery of lithium from the cathodes of spent NMC batteries through the hydrometallurgical process using a sodium hydroxide solution. The leaching process was carried out in 2 M and 4 M NaOH concentrations for 120 minutes at high pressure and at temperatures of 398.15 K, 423.15 K, 448.15 K, and 473.15 K. Experimental results showed that 56.53% of lithium could be recovered with nearly 100% selectivity under the optimum leaching conditions of 473.15 K and 4 M NaOH. The release of lithium ions was due to a combination of sodium adsorption, ion exchange, and impregnation mechanisms. Result: Calculation results showed that the activation energy of the lithium leaching process was 2.1990×104 J/mol, the reaction was endothermic with enthalpy and entropy at standard conditions (298.15 K) of 4.8936×105 J/mol and 1.4421×103 J/mol/K, respectively. Conclusion: The present work also suggested that total lithium recovery can be increased through a series of leaching processes.

A mild and efficient closed-loop recycling strategy for spent lithium-ion battery

As lithium metal resource supply and demand stabilize and prices decrease, the efficient recovery of valuable metals other than lithium from spent lithium-ion batteries is receiving increasing attention. Currently, challenges remain in the selective lithium recovery efficiency and the high cost of regenerating valuable metal slag after lithium extraction, particularly for spent ternary cathode materials. To address these challenges, this study introduces a closed-loop recovery process for spent ternary cathode materials, employing sulfur-assisted roasting to achieve efficient lithium extraction and high-value direct regeneration of ternary leaching residues. At moderate temperatures (500 ℃), LiNixCoyMn1−x-yO2 (NCM) materials undergo a directional transformation of lithium to Li2SO4 in synergy with sulfur and oxygen, achieving a lithium leaching extraction rate of 98.91 %. Additionally, the relatively mild reaction conditions preserve the secondary spherical morphology and uniform distribution of NiCoMn-based oxide residue without introducing adverse impurities, ensuring the successful regeneration of high-value NCM cathode materials (R-NCM). The R-NCM material exhibits good discharge capacity (144.3 mA·h/g at 1 C) and relatively stable cycling performance, with a capacity retention rate of 80 % after 150 cycles. This work provides a viable pathway for the efficient and environmental-friendly pyrometallurgical closed-loop recovery of spent lithium-ion batteries.

Selective Solid-Liquid Extraction of Lithium Cation Using Tripodal Sulfate-Binding Receptors Driven by Electrostatic Interactions.

Owing to the important role of and increasing demand for lithium resources, lithium extraction is crucial. The use of molecular extractants is a promising strategy for selective lithium recovery, in which the interaction between lithium and the designed extractant can be manipulated at the molecular level. Herein, we demonstrate that anion receptors of tripodal hexaureas can selectively extract Li2SO4 solids into water containing DMSO (0.8% water) compared to other alkali metal sulfates. The hexaurea receptor with terminal hexyl chains displays the best Li+ extraction selectivity at 2-fold over Na+ and 12.5-fold over K+. The driving force underpinning selective lithium extraction is due to the combined interactions of Li+-SO42- electrostatics and the ion-dipole interaction of the lithium-receptor (carbonyl groups and N atoms); the latter was found to be cation size dependent, as supported by computational calculations. This work indicates that anion binding receptors could drive selective cation extraction, thus providing new insights into the design of receptors for ion recognition and separation.

In-situ oxidation for selective lithium extraction from spent LiFePO4 cathodes by low acid dosage

Recovery of lithium from spent lithium iron phosphate batteries is crucial to alleviating the storage of lithium. This study proposes a method for the selective recovery of lithium from spent lithium iron phosphate battery cathodes using a leaching system of H2SO4 and H2O2. Efficient and selective lithium recovery was achieved through in-situ oxidation of lithium iron phosphate driven by a low acid dosage, and the mechanism of selective lithium recovery was investigated by precipitation experiments of Fe2+ and PO43−. The shrinking core model was used for the kinetic analysis of the leaching process, and the results suggested that the leaching process was controlled by the internal diffusion of the product layer. Moreover, essential leaching parameters such as acid concentration, H2SO4 dosage, H2O2 dosage, leaching time, and leaching temperature were systematically investigated. The results showed that the leaching rate of Li reached 97.95 % along with a selectivity of 99.60 %, which meets the standard of the battery-grade Li2CO3, while the leaching rate of both Fe and P was less than 1 %.

Selective lithium extraction employing lithium manganese oxide-loaded polymeric membranes at natural brine pH and room temperature

The current technology for lithium extraction from brines is recognized both for its techno-economic disadvantages and its environmental impacts. We have synthesized, characterized, and evaluated particles based on lithium manganese oxide towards selective lithium recovery from complex media. A solid-state synthesis and a hydrothermal method produced sub-micrometre sized particles that showed diameters of 253 nm and 154 nm, respectively, both with very low polydispersity. 23.7 mgLi/gHMO and 30.7 mgLi/gHMO adsorption capacity values were obtained with solid-state synthetic and hydrothermal oxides. The hydrothermally synthesized sub-micrometre sized particles were incorporated into polymeric membranes aiming at the development of a straightforward technological application. Membranes were prepared from polyacrylonitrile and polyethylene-glycol, and the affinity to lithium was once again evaluated. Membranes showed a high adsorption capacity for lithium (32.7 mgLi/gHMO) with almost identical kinetics and cyclability as the free particles in solution. An excellent selectivity for lithium was confirmed in experiments with a natural lithium-rich brine from the Lithium Triangle. All adsorption experiments were performed at neutral pH and room temperature. An undeniable advantage of membranes vs. sub-micrometre sized particles is that the former do not require centrifugation after successful adsorption/desorption. These three characteristics are fundamental in the perspective of technology scale-up to minimize operational costs.

Selective recovery of lithium from spent LiFePO4 powders with electrochemical method

In recent years, with the flourishing of new energy vehicles, the lithium iron phosphate (LFP) batteries are vigorously developed due to their low cost and high stability. Meanwhile, it leads to an increase in large-scale retirement of batteries. Therefore, it is crucial to develop a green and efficient recycling method. In this work, an indirect electrochemical oxidation has been proposed for selective leaching of Li ions. An electrochemical system using boron-doped diamond electrode (BDD) with high oxygen evolution potential as anode and RuO2/Ti as cathode has been built to generate oxidizing species and enhance the oxidative reaction contact for an indirect oxidation of LFP. The operating conditions were optimized to a current density of 110 mA/cm2, Na2SO4 electrolyte concentration of 0.225 M, pH of 1.7, solid–liquid ratio of 16 g/L. The leaching efficiency of Li ions reached up to 95.53 % and the leaching efficiency of Fe ions was less than 0.01 % at room temperature. A purity of lithium carbonate product of 99.93 % was obtained after precipitation of the leaching solution. This proposed method could realize efficient and rapid selective leaching of Li and Fe ions by indirect oxidation, realizing selective leaching and significantly reducing the usage of acid.

Novel targeted extraction of lithium: An environment-friendly controlled sulfidation roasting technology and mechanism for recovering spent lithium-ion batteries

Due to the needs of protecting the environment and recycling resources, the extraction of lithium from spent lithium-ion batteries has become increasingly important. Different from the traditional roasting process, a novel approach for the selective recovery of lithium from spent LiCoO2 (SLCO) through low-temperature sulfidation roasting was proposed in the present work. The thermodynamics of the sulfidation roasting was investigated and phase transformation was detected. The results showed that the S2 gas generated from the decomposition of pyrite converted LiCoO2 into Li2SO4 and cobalt sulfides. Under optimal experimental conditions, lithium can be selectively leached with a yield of more than 99% through water immersion treatment, resulting in around 20% improvement in the overall recovery rate of the metal compared to current industrial practices. The thermochemical process did not produce toxic SOx gases, whereas the selective leaching process for lithium did not require additional reagents, resulting in good environmental and economic benefits.

Preferentially selective recovery of lithium from spent LiCoO2 by sulfation roasting of MnSO4

The selective recovery of valuable metals from spent lithium-ion batteries (LIBs) has engrossed significant scientific attention due to prompting environmental potential and addressing resource scarcity. Hereby, we propose an innovative and economically more environment friendly manganese sulfate roasting water leaching process to selectively recuperate lithium preferentially from spent LiCoO2 batteries. Notably, it is found that manganese sulfate roasting agents can be recirculated thoroughly without SOx emission during the sulfation roasting process. To better understand the conversion mechanism of LiCoO2, the effects of numerous parameters including, roasting time, roasting temperature, and a molar ratio of MnSO4/LiCoO2 during the recovering process were investigated. An exceptional recovery rate of 98.62% with a remarkable lithium selectivity of 99.35% by manganese sulfate leaching was achieved. This work proposes an environmentally friendly and promising strategy to extract lithium selectively from spent lithium cathodes without introducing SOx emission.

Dialkyl(5-ethyl-2-hydroxyphenyl)phosphonates as extractants for the selective recovery of lithium from alkaline media

Dialkyl(5-ethyl-2-hydroxyphenyl)phosphonates as extractants for the selective recovery of lithium from alkaline media

A green recycling process for spent lithium-ion batteries with extremely low chemical consumption

Selective recovery of lithium from spent cathodes is an attractive, green and efficient recycling method for spent lithium-ion batteries (LIBs). However, current technologies face numerous challenges including high reagent consumption, limited versatility and significant secondary pollution. In this study, we found that an intermediate phase formed during leaching exhibited high physiochemical stability, which hindered leaching of Li+ and led to increased reagent and energy consumption. A simple mechanical activation strategy was used to change the intermediate phase of the leaching process by activating the spent cathode without grinding additives. The energy input of the mechanical force resulted in defects in the activated waste, leading to a novel activated intermediate phases. Through experimental characterization and DFT analyses, this novel intermediate phase containing H+ was found to have a large specific surface area, large internal stress and low reaction energy, which enabled the leaching of the Li+. As a result, the method showed a high utilization efficiency of H+ in recycling most spent cathodes. In the end, we established a closed-loop recovery route for spent LIBs that exhibited exceptional efficiency for H+ utilization (> 97 %), obviated the need for auxiliary reagents, and substantially reduced secondary pollutant generation.

A high-efficiency and low-carbon strategy for selective lithium recovery from spent lithium-ion batteries: Combining mechanochemical activation with biomass reduction roasting

Biomass reduction roasting has attracted considerable attention as an emerging strategy for selectively recovering lithium from spent lithium-ion batteries (LIBs). However, the utilization of excessive roasting conditions in current practices results in significant energy consumption and C emissions, thereby hindering further development. Herein, we propose a novel recycling strategy that combines mechanochemical activation (MCA) with biomass reduction roasting. The optimized roasting conditions with MCA pretreatment achieve a 100 °C reduction in roasting temperature, a halving of biomass ratio and roasting time, compared to the case without activation. By analyzing the changes in physicochemical properties of mixed samples (cathode materials and biomass) under different activation conditions and their impacts, the action mechanism of MCA on biomass reduction roasting is revealed. The introduction of MCA pretreatment achieves milder roasting conditions by promoting homogeneous mixing and disrupting NCM crystal structures through the “pre-oxygen elements removal” process. Furthermore, mechanical treatment was applied to enhance the carbonated water leaching process. The results of sustainability analysis and economic evaluation demonstrate that the proposed recycling strategy not only reduces CO2 emissions and energy consumption but also generates considerable benefits. Overall, this high-efficiency and low-carbon recycling strategy provides a promising direction for the development of spent LIBs recycling technology.