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While many nutrient recovery technologies target liquid waste streams, new strategies are required for effective phosphorus recovery from solid waste. This study reports an innovative ligand-enabled Donnan dialysis process to recover orthophosphate (P(V)) from alum-laden waste activated sludge (WAS). Four ligands, namely acetate, citrate, ethylenediaminetetraacetate (EDTA), and oxalate, were evaluated for P(V) release from a synthetic sludge containing 5 mM P(V) and 25 mM Al(III) and a real, alum-laden WAS with similar contents. Citrate and EDTA released more than 95% of P(V) at doses of 30 mM, outperforming acetate and oxalate. The ligand-based solubilization strategy was coupled with Donnan dialysis to recover P(V) into a clean sodium chloride draw solution. After Donnan dialysis with the synthetic sludge, the P(V) recovery's order was as follows: EDTA (54.4%) > citrate (41.7%) > oxalate (4.3%). The P(V) recovery efficiencies were slightly lower for Donnan dialysis with real, alum-laden WAS, namely 45.1% and 25.2% for EDTA and citrate addition, respectively, due to competitive effects exerted by other dissolved species. These promising results successfully demonstrated the proof-of-concept for ligand-enabled Donnan dialysis.