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Phase diagrams, thermal stabilities and the mechanism of thermal decomposition are reported, along with densities and insights from 31P NMR spectroscopic studies. The work was concluded with a proof-of-concept demonstration of the use of the TOPOmalonic acid (2  1 mol ratio) mixture for the extraction of gallium from acidic chloride feedstock (simulated pre-digestate of zinc leach residue). The loading capacity of the TOPOmalonic acid extractant was three orders of magnitude greater than that of the literature benchmark, encouraging fur