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This work reports a mechanochemical (MC) method for complete defluorination of perfluorooctanoic acid (PFOA) by using Al and Al2O3 as milling agents. Both the Al/Al2O3 molar ratio ( [Formula see text] ) and the pre-thermal treatment of Al2O3 strongly influenced the defluorination of PFOA. When commercial γ-Al2O3 was pre-treated at 1200 °C, the use of Al and heat-treated γ-Al2O3 with [Formula see text] of 1 1 led to PFOA defluorination of 100% after ball milling for 26 min at 350 rpm, being much higher than those (8.3%-58.1%) for using si