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

K. Jayanthi; Mariappan Parans Paranthaman; Benjamin T. Manard; Alexandra Navrotsky

doi:10.1021/acs.jpcc.3c05676

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

K. Jayanthi, Mariappan Parans Paranthaman, Benjamin T. Manard, Alexandra Navrotsky

Research output: Contribution to journal › Article › peer-review

5 Scopus citations

Abstract

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. 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.

Original language	English
Pages (from-to)	23879-23886
Number of pages	8
Journal	Journal of Physical Chemistry C
Volume	127
Issue number	49
DOIs	https://doi.org/10.1021/acs.jpcc.3c05676
State	Published - Dec 14 2023

Funding

This research was supported by the Critical Materials Institute, an Energy Innovation Hub funded by the US Department of Energy (Subaward no. DEAC05-00OR22725), and (Subaward no. DE-AC02-07CH11358) Office of Energy Efficiency and Renewable Energy, Advanced Materials and Manufacturing Technologies Office. The synthesis of LDH sorbents was supported by the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Office of Geothermal Technologies Office through a Technology Commercialization Fund. This manuscript has been authored by UT-Battelle, LLC under contract no. DEAC05-00OR22725 with the U.S. Department of Energy.

Funders	Funder number
Critical Materials Institute
Office of Geothermal Technologies Office
U.S. Department of Energy	DE-AC02-07CH11358, DEAC05-00OR22725
Office of Energy Efficiency and Renewable Energy
Advanced Materials and Manufacturing Technologies Office

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title = "Effect of Anions on the Delithiation of [Li-Al] Layered Double Hydroxides: Thermodynamic Insights",

abstract = "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 SO42-), which were synthesized and dried under different conditions. 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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AB - 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 SO42-), which were synthesized and dried under different conditions. 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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Effect of Anions on the Delithiation of [Li-Al] Layered Double Hydroxides: Thermodynamic Insights

Abstract

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