The dissolution mechanism of S-phase particles in 2024-T351 aluminum alloy at open-circuit potential in chloride-containing sulfate solutions was investigated using atomic force microscopy (AFM), scanning Kelvin probe force microscopy (SKPFM), and secondary ion mass spectroscopy (SIMS). The combination of the three techniques allowed the correlation between SKPFM measurements and the corrosion behavior of AA2024 to be confirmed, leading to a better understanding of the electrochemical behavior of S-phase particles. A three-step mechanism for the dissolution and accompanying processes occurring near S particles was proposed: (i) preferential aluminum and magnesium dissolution, (ii) galvanic coupling between the copper-enriched particles and the surrounding matrix, leading to an increased passivity of the matrix around the particles, and (iii) copper deposition around the corroded particles. (c) 2008 The Electrochemical Society.