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Advanced oxidation technologies often use peroxymonosulfate in the presence of CoIIaq. It is commonly assumed that the reaction of Co(H2O)62+ with HSO5− yields CoIIIaq and SO4.−. DFT results point out that first CoII(SO5)(H2O)2 is formed. The homolysis of CoII(SO5)(H2O)2 to yield (H2O)CoII(SO5)OH.+SO4.−, is exothermic but has a large activation energy. However the cobalt is not oxidized in this reaction...