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Integrated Circular Economy Model System for Direct Lithium Extraction: From Minerals to Batteries Utilizing Aluminum Hydroxide
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    Integrated Circular Economy Model System for Direct Lithium Extraction: From Minerals to Batteries Utilizing Aluminum Hydroxide
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    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2023, 15, 50, 58984–58993
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    https://doi.org/10.1021/acsami.3c12070
    Published December 5, 2023
    Copyright © 2023 American Chemical Society

    Abstract

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    Aluminum hydroxide, an abundant mineral found in nature, exists in four polymorphs: gibbsite, bayerite, nordstrandite, and doyleite. Among these polymorphs gibbsite, bayerite, and commercially synthesized amorphous aluminum hydroxide have been investigated as sorbent materials for lithium extraction from sulfate solutions. The amorphous form of Al(OH)3 exhibits a reactivity higher than that of the naturally occurring crystalline polymorphs in terms of extracting Li+ ions. This study employed high-temperature oxide melt solution calorimetry to explore the energetics of the sorbent polymorphs. The enthalpic stability order was measured to be gibbsite > bayerite > amorphous Al(OH)3. The least stable form, amorphous Al(OH)3, undergoes a spontaneous reaction with lithium, resulting in the formation of a stable layered double hydroxide phase. Consequently, amorphous Al(OH)3 shows promise as a sorbent material for selectively extracting lithium from clay mineral leachate solutions. This research demonstrates the selective direct extraction of Li+ ions using amorphous aluminum hydroxide through a liquid–solid lithiation reaction, followed by acid-free delithiation and relithiation processes, achieving an extraction efficiency of 86%, and the maximum capacity was 37.86 mg·g–1 in a single step during lithiation. With high selectivity during lithiation and nearly complete recoverability of the sorbent material during delithiation, this method presents a circular economy model. Furthermore, a life cycle analysis was conducted to illustrate the environmental advantages of replacing the conventional soda ash-based precipitation process with this method, along with a simple operational cost analysis to evaluate reagent and fuel expenses.

    Copyright © 2023 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsami.3c12070.

    • Elemental mapping images, plot of relative pressure (P/Po) vs quantity adsorbed (cm2/g STP) for A-Al(OH)3 and A-SO4-LDH, PXRD patterns and FTIR spectra of gibbsite, bayerite, and amorphous aluminum hydroxides, crystal structure of gibbsite and bayerite viewed down the b axes, kinetics experiment results depicting the percentage of Li uptake from the simulant by stoichiometric A-Al(OH)3 with respect to time, ICP OES results of the supernatant obtained after the lithiation process (ppm = μg/mL) in the kinetic experiments, and formula to calculate the loading of Li in the solid sample (PDF)

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    This article is cited by 6 publications.

    1. Priyesh Wagh, Syed Z. Islam, Tej Nath Lamichhane, Ramesh R. Bhave, Mariappan Parans Paranthaman. Separation of Lithium from Aluminum-Containing Clay Mineral Leachate Solution Using Energy-Efficient Membrane Solvent Extraction. ACS Omega 2023, 8 (49) , 46523-46527. https://doi.org/10.1021/acsomega.3c05009
    2. Venkat Roy, Mariappan Parans Paranthaman, Fu Zhao. Lithium from clay: Assessing the environmental impacts of extraction. Sustainable Production and Consumption 2024, 52 , 324-332. https://doi.org/10.1016/j.spc.2024.11.008
    3. Sabbir Ahmed, Anil Kumar Madikere Raghunatha Reddy, Karim Zaghib. Transformations of Critical Lithium Ores to Battery-Grade Materials: From Mine to Precursors. Batteries 2024, 10 (11) , 379. https://doi.org/10.3390/batteries10110379
    4. Muhammed Rashik Mojid, Kyung Jae Lee, Jiahui You. A review on advances in direct lithium extraction from continental brines: Ion-sieve adsorption and electrochemical methods for varied Mg/Li ratios. Sustainable Materials and Technologies 2024, 40 , e00923. https://doi.org/10.1016/j.susmat.2024.e00923
    5. Conglin You, Dongdong Li, Yanfei Fan, Dandan Gao, Li Han, Dewen Zeng. Rationalize the High Performance of Lithium Sorbents Derived from Gibbsite Guided by Phase Chemistry. Journal of Sustainable Metallurgy 2024, 10 (2) , 893-902. https://doi.org/10.1007/s40831-024-00839-w
    6. Tao Wang, Huimin Luo, Yaocai Bai, Ilias Belharouak, K. Jayanthi, Mariappan Parans Paranthaman, Benjamin T. Manard, Evelyna Tsi-Hsin Wang, Fulya Dogan, Seoung-Bum Son, Brian J. Ingram, Qiang Dai, Sheng Dai. Direct recycling of spent nickel-rich cathodes in reciprocal ternary molten salts. Journal of Power Sources 2024, 593 , 233798. https://doi.org/10.1016/j.jpowsour.2023.233798
    7. Venkat Roy, M. Parans Paranthaman, Fu Zhao. Lithium from Clay: Assessing the Environmental Impacts of Extraction. 2024https://doi.org/10.2139/ssrn.4782093

    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2023, 15, 50, 58984–58993
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsami.3c12070
    Published December 5, 2023
    Copyright © 2023 American Chemical Society

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