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Ensuring continuous and sustainable lithium supply requires the development of highly efficient separation processes such as LLE (liquid‐liquid extraction) for both primary sources and certain waste streams. In this work, 4‐phosphoryl pyrazolones are used in an efficient pH‐controlled stepwise separation of Li+ from Ca2+, Mg2+, Na+ and K+. The factors affecting LLE process, such as the substitution pattern of the extractant, diluent/water distribution, co‐ligand, pH, and speciation of the metal complexes involved, were systematically investigated. The maximum extraction efficiency of Li+ at pH 6.0 was 94 % when Mg2+ and Ca2+ were previously separated at pH<5.0, proving that the separation of these ions is possible by simply modulating the pH of the aqueous phase. Our study points a way to separation of lithium from acid brine or from spent lithium ion battery leaching solutions, which supports the future supply of lithium in a more environmentally friendly and sustainable manner. [ABSTRACT FROM AUTHOR]

Keywords: Ca/Mg/Li Separation; Di- and Trinuclear Complexes; Separation Science; pH-Regulated Receptors; 4-Phosphoryl Pyrazolone Ligands EN Ca/Mg/Li Separation Di- and Trinuclear Complexes Separation Science pH-Regulated Receptors 4-Phosphoryl Pyrazolone Ligands 1 1 1 03/15/23 20230320 NES 230320 B Receptors b . Ca/Mg/Li Separation, Di- and Trinuclear Complexes, Separation Science, pH-Regulated Receptors, 4-Phosphoryl Pyrazolone Ligands Frontispiece: Selective Separation of Lithium, Magnesium and Calcium using 4-Phosphoryl Pyrazolones as pH-Regulated Receptors. [Extracted from the article]