Novel Positively Charged Metal-Coordinated Nanofiltration Membrane for Lithium Recovery

Wang, Li; Rehman, Danyal; Sun, Pengfei; Deshmukh, Akshay; Zhang, Liyuan; Han, Qi; Yang, Zhe; Wang, Zhongying; Park, Hee Deung; Lienhard, John H.; Tang, Chuyang Y.

doi:10.1021/acsami.1c02252

Cited by 93 publications

(37 citation statements)

References 65 publications

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“…The flexibility of the superstructure model allows it to systematically explore the vast design space associated with the development of higher selectivity membranes. For example, Figure shows nanofiltration membranes (α = 10–30) can improve recoveries of both species using less membrane area when compared to low selectivity membranes (α = 2.6). , (The selectivity α is a key membrane performance parameter in the optimization models described in the Methods.) Because of the smaller module size required, these membranes simplify the design of the system significantly when compared to a poor selectivity membrane.…”

Section: Resultsmentioning

confidence: 99%

Optimal Diafiltration Membrane Cascades Enable Green Recycling of Spent Lithium-Ion Batteries

Wamble

Eugene

Phillip

et al. 2022

ACS Sustainable Chem. Eng.

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Novel processes are urgently needed to recycle critical materials (e.g., cobalt, lithium, nickel, and manganese) from spent lithium-ion batteries (LIBs). These separations are vital both to meet growing global demand and to mitigate a looming e-waste crisis. Currently, to recover cobalt and lithium from spent LIBs, high temperatures and organic solvents are used to separate Co2+ and Li+ in complex leaching and extraction processes. In contrast to using expensive designer ligands or harmful organic solvents, this work reveals that continuous membrane cascades are a promising aqueous-based alternative to recover these critical materials and facilitate their reuse. A superstructure optimization model that designs diafiltration cascades to maximize material recovery and purity as a function of membrane material performance and feed specifications is developed. This approach enables the comparison of candidate membrane materials by rapidly predicting the Pareto optimal trade-offs between the recovery and purity of lithium and cobalt for bespoke cascade designs. For example, the model predicts that, when deployed in an optimized two-stage cascade configuration, a nanofiltration membrane with a modest selectivity of 32 can be used to recover 95% Li+ and 99% Co2+ at 93 and 99.5 wt % purity, respectively. On the basis of analysis of over 1000 Pareto optimal designs, six design heuristics for executing binary separations using staged diafiltration cascades are proposed. Moreover, by evaluating membrane materials in the context of optimized diafiltration processes, this work quantifies the benefits of materials improvements and shows that the greatest research opportunities for membrane-based LIB recycling are at the device and systems scales. More broadly, the optimization models represent a robust framework for identifying the most effective way to deploy emerging materials in integrated process systems. This transformative capability is widely applicable to many of the separations needed to support sustainable global development.

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Section: Resultsmentioning

confidence: 99%

Optimal Diafiltration Membrane Cascades Enable Green Recycling of Spent Lithium-Ion Batteries

Wamble

Eugene

Phillip

et al. 2022

ACS Sustainable Chem. Eng.

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“…[165,166] Positively charged NF membranes were also investigated and showed a superior attitude in the separation of Li + /Mg 2+ ions in highly concentrated streams due to the Donnan exclusion phenomenon. [167][168][169][170][171][172][173][174]…”

Section: Nanofiltration Membranesmentioning

confidence: 99%

Recent Advances in the Lithium Recovery from Water Resources: From Passive to Electrochemical Methods

et al. 2022

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The ever-increasing amount of batteries used in today's society has led to an increase in the demand of lithium in the last few decades. While mining resources of this element have been steadily exploited and are rapidly depleting, water resources constitute an interesting reservoir just out of reach of current technologies. Several techniques are being explored and novel materials engineered. While evaporation is very time-consuming and has large footprints, ion sieves and supramolecular systems can be suitably tailored and even integrated into membrane and electrochemical techniques. This review gives a comprehensive overview of the available solutions to recover lithium from water resources both by passive and electrically enhanced techniques. Accordingly, this work aims to provide in a single document a rational comparison of outstanding strategies to remove lithium from aqueous sources. To this end, practical figures of merit of both main groups of techniques are provided. An absence of a common experimental protocol and the resulting variability of data and experimental methods are identified. The need for a shared methodology and a common agreement to report performance metrics are underlined.

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“…Thanks to their energy efficiency, application facility and ecological sustainability, membrane technologies have attracted wide interest for lithium procurement using different membrane processes such as Nanofiltration [30,31], Reverse Osmosis (RO) [32], Dialysis [33] and Electrodialysis (ED) [34,35]. For efficient extraction and optimal product quality, the used membranes need to exhibit a specific selectivity towards Li + compared to other existent cations.…”

Section: Introductionmentioning

confidence: 99%

Lithium-Sodium Separation by a Lithium Composite Membrane Used in Electrodialysis Process: Concept Validation

et al. 2022

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The recent expansion of global Lithium Ion Battery (LIBs) production has generated a significant stress on the lithium demand. One of the means to produce this element is its extraction from different aqueous sources (salars, geothermal water etc.). However, the presence of other mono- and divalent cations makes this extraction relatively complex. Herein, we propose lithium-sodium separation by an electrodialysis (ED) process using a Lithium Composite Membrane (LCM), whose effectiveness was previously demonstrated by a Diffusion Dialysis process (previous work). LCM performances in terms of lithium Recovery Ratio (RR(Li+)) and Selectivity (S(Li/Na)) were investigated using different Li+/Na+ reconstituted solutions and two ED cells: a two-compartment cell was chosen for its simplicity, and a four-compartment one was selected for its potential to isolate the redox reactions at the electrodes. We demonstrated that the four-compartment cell use was advantageous since it provided membrane protection from protons and gases generated by the electrodes but that membrane selectivity was negatively affected. The impact of the applied current density and the concentration ratio of Na+ and Li+ in the feed compartment ([Na+]F/[Li+]F) were tested using the four-compartment cell. We showed that increasing the current density led to an improvement of RR(Li+) but to a reduction in the LCM selectivity towards Li+. Increasing the [Na+]F/[Li+]F ratios to 10 had a positive effect on the membrane performance. However, for high values of this ratio, both RR(Li+) and S(Li/Na) decreased. The optimal results were obtained at [Na+]F/[Li+]F near 10, where we succeeded in extracting more than 10% of the initial Li+ concentration with a selectivity value around 112 after 4 h of ED experiment at 0.5 mA·cm−2. Thus, we can objectively estimate that the concept of this selective extraction of Li+ from a mixture even when concentrated in Na+ using an ED process was validated.

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Novel Positively Charged Metal-Coordinated Nanofiltration Membrane for Lithium Recovery

Cited by 93 publications

References 65 publications

Optimal Diafiltration Membrane Cascades Enable Green Recycling of Spent Lithium-Ion Batteries

Optimal Diafiltration Membrane Cascades Enable Green Recycling of Spent Lithium-Ion Batteries

Recent Advances in the Lithium Recovery from Water Resources: From Passive to Electrochemical Methods

Lithium-Sodium Separation by a Lithium Composite Membrane Used in Electrodialysis Process: Concept Validation

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