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The corrosion behavior of 3A21 aluminum alloy in different concentrations of ethylene glycol solution under different simulated atmospheres was studied by electrochemical methods (potentiodynamic polarization and electrochemical impedance spectroscopy) and surface analytical techniques (metalloscopy and the scanning electron microscope equipped with energy-dispersive x-ray spectrometer). The electrochemical results showed that the corrosion of 3A21 aluminum alloy was affected by the concentration of ethylene glycol solution and atmosphere conditions, and the influence of atmosphere was different in different concentrations of ethylene glycol solution. The results were further confirmed by morphology analysis, and the formation of Al-alcoholized film on the surface of aluminum alloy was proved by element energy spectrum analysis, then the corrosion mechanism of 3A21 aluminum alloy was discussed.