Effect of Anions on the Delithiation of [Li–Al] Layered Double Hydroxides: Thermodynamic Insights

Jayanthi, Kumar; Paranthaman, Mariappan Parans; Manard, Benjamin T.; Navrotsky, Alexandra

doi:10.1021/acs.jpcc.3c05676

Title: Effect of Anions on the Delithiation of [Li–Al] Layered Double Hydroxides: Thermodynamic Insights

Journal Article · 04 December 2023 · Journal of Physical Chemistry. C

DOI: https://doi.org/10.1021/acs.jpcc.3c05676 · OSTI ID:2281983

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Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Arizona State Univ., Tempe, AZ (United States)

The utilization of lithium aluminum [Li–Al] layered double hydroxides (LDHs) is explored for direct lithium extraction (DLE) from geothermal brines and minerals. Following extraction, the Li⁺ ions need to be removed from the LDH structure and converted into LiOH or Li²CO³ products, making them suitable for battery applications. The research investigates the delithiation of [Li–Al-X] LDHs (where X = Cl^–, OH^–, and SO₄^2–), which were synthesized and dried under different conditions. Herein the study aims to understand how the choice of anions and drying conditions affects the delithiation process. To determine the stability of these [Li–Al] LDHs, high-temperature oxide melt solution calorimetry is employed. The results reveal that the stability of LDHs varies significantly based on postdrying conditions, anion choice, and the water content in the interlayer. The order of stability, as indicated by the enthalpy of formation values, is found to be OH-LDH-O > OH-LDH-A > SO₄-LDH-O > SO4-LDH-A > Cl-LDH-O > Cl-LDH-A. This trend is attributed to the interactions among the interlayer species and the metal hydroxide layers.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Energy Efficiency Office. Advanced Materials & Manufacturing Technologies Office (AMMTO); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Renewable Power Office. Geothermal Technologies Office

Grant/Contract Number:: AC05-00OR22725; AC02-07CH11358

OSTI ID:: 2281983

Journal Information:: Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 49 Vol. 127; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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