Two ionic liquid (IL) thermomorphic systems were designed. The thermoregulated property exhibited by the IL systems was utilized for the recovery of Au(III) from acidic medium. The cloud point order of the two ILs was proposed and evidenced via a combination of experimental measurements and quantum chemical calculations. The impacts of salt ions and acid on the thermomorphic phase behavior of the IL–H₂O binary mixture system were investigated. After comprehensive comparison, a systematic study of Au(III) extraction by the [Suc][Tf₂N]₂ (succinyl bis(trifluoromethylsulfonyl)imide) system was carried out because of its outstanding hydrophobicity and extraction ability. Then, a comparison between traditional liquid–liquid extraction (TLLE) and homogeneous liquid–liquid extraction (HLLE) was made during the process of optimization of various extraction parameters. In addition, the anion-exchange mechanism in the extraction process was revealed. The thermoregulated [Suc][Tf₂N]₂ system presented an excellent selectivity for Au(III) in a solution of coexisting multimetallic ions. Finally, Au(III) was almost completely stripped from the loaded IL phase by oxalic acid. The extraction efficiency of Au(III) using regenerated IL still maintains a surprising stability after five turns of cycling experiments. Hence, the dicationic IL [Suc][Tf₂N]₂ was regarded as a potential extractant for the recovery of gold.
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