Lithium Carbonate Conversion to Lithium Hydroxide Using Calcium Hydroxide: Equilibrium is Governed by Vaterite Formation

Torok, Peter and Halasine-Varga, Ilona and Duvivier, Laurent and Maimi, Maha and Hubert, Olivier and Minnaar, Susanna and Sipos, Pál Miklós and du, Plessis Chris and Kutus, Bence (2025) Lithium Carbonate Conversion to Lithium Hydroxide Using Calcium Hydroxide: Equilibrium is Governed by Vaterite Formation. INORGANIC CHEMISTRY, 64 (48). pp. 23575-23585. ISSN 0020-1669

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Abstract

The conversion of lithium carbonate (Li2CO3) with calcium hydroxide (Ca(OH)2) is a cornerstone industrial process for synthesizing lithium hydroxide (LiOH), a critical precursor for high-performance cathodes in advanced lithium-ion batteries. Achieving a high Li2CO3-to-LiOH yield is crucial for efficient industrial processing. However, despite its industrial relevance, the influence of concentration and equilibrium conditions on this conversion reaction remains insufficiently explored. To address this gap, we investigated the conversion reaction by varying the Li2CO3 concentration and the Ca(OH)2:Li2CO3 molar ratio. Near-complete conversion yields occur below the maximum concentration threshold of 1.6 mol L-1 LiOH, while yields diminish above this limit. Sequential reaction experiments confirm that the system adheres to Le Chatelier's principle, and reverse reactions initiated from LiOH and CaCO3 demonstrate true equilibrium behavior. Furthermore, backward reactions involving distinct CaCO3 polymorphs reveal different equilibrium states. Notably, the presence of vaterite alongside calcite significantly affects the equilibrium concentration of LiOH, underscoring the role of solid-phase composition in governing reaction thermodynamics. These findings provide a deeper understanding of the causticization mechanism and offer actionable insights for optimizing LiOH production in industrial settings.

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