Integrated Circular Economy Model System for Direct Lithium Extraction: From Minerals to Batteries Utilizing Aluminum Hydroxide

K. Jayanthi, Tej N. Lamichhane, Venkat Roy, Fu Zhao, Alexandra Navrotsky, Bruce A. Moyer, Mariappan Parans Paranthaman

Research output: Contribution to journalArticlepeer-review

5 Scopus citations

Abstract

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.

Original languageEnglish
Pages (from-to)58984-58993
Number of pages10
JournalACS Applied Materials and Interfaces
Volume15
Issue number50
DOIs
StatePublished - Dec 20 2023

Funding

Thanks are due to Benjamin T Manard and Barbara Evans for help with ICP-OES measurements. Scanning electron microscopy (SEM) microstructural characterizations were conducted a part of a user project at the Center for Nanophase Materials Sciences (CNMS), which is a U.S. Department of Energy Office of Science User Facility at Oak Ridge National Laboratory. Thanks are due to Dale Hensley for help with SEM measurements. This research was supported by the Critical Materials Institute, an Energy Innovation Hub funded by the U.S. Department of Energy (Subaward Number DEAC05-00OR22725), Office of Energy Efficiency and Renewable Energy’s Advanced Materials and Manufacturing Technologies Office. Part of the lithium extraction research (M.P.P.) was performed through the Re-Cell Center, which gratefully acknowledges support from the U.S. Department of Energy (DOE), Office of Energy Efficiency and Renewable Energy, and the Vehicle Technologies Office. Thanks are due to Arvind Ganesan for helping with pore structure characterization and BET measurement. This manuscript has been authored by UT-Battelle, LLC under Contract no. DEAC05-00OR22725 with the U.S. Department of Energy.

FundersFunder number
Critical Materials Institute
Office of Energy Efficiency and Renewable Energy’s Advanced Materials and Manufacturing Technologies Office
U.S. Department of EnergyDEAC05-00OR22725
Office of Science
Office of Energy Efficiency and Renewable Energy
Oak Ridge National Laboratory

    Keywords

    • aluminum hydroxide
    • amorphous
    • circular economy
    • delithiation
    • direct lithium extraction
    • lithiation
    • relithiation

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