Dissolution of elemental gold in organic solutions is ac ontemporary approach to lower the environmental burden associated with gold recycling.Herein, we describe fundamental studies on ah ighly efficient method for the dissolution of elemental Au that is based on DMF solutions containing pyridine-4-thiol (4-PSH) as ar eactive ligand and hydrogen peroxidea sa no xidant. Dissolution of Au proceeds through several elementary steps:i somerization of 4-PSH to pyridine-4-thione (4-PS), coordination with Au 0 ,and then oxidation of the Au 0 thione species to Au I simultaneously with oxidation of free pyridine thione to elemental sulfur and further to sulfuric acid. The final dissolution product is aA u I complex bearing two 4-PS ligands and SO 4 2À as ac ounterion. The ligand is crucial as it assists the oxidation process and stabilizes and solubilizes the formed Au cations.