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The interfacial bonding and the layered structure of 2-mercaptobenzimidazole (2-MBI) organic films adsorbed on electrochemically controlled copper surfaces and their corrosion inhibition effects in acidic chloride aqueous solution were investigated using an integrated approach of electrochemical methods and advanced surface analyses by X-ray photoelectron spectroscopy and time-of-flight secondary ion mass spectrometry. It is shown that organic films formed on the copper surfaces are bi-layered with a chemisorbed inner layer and a physisorbed outer layer. In the chemisorbed inner layer, 2-MBI is bonded primarily by its nitrogen atoms with metallic and oxidized copper surfaces. Sulphur atoms are also involved in the bonding mechanism when metallic copper is directly accessible to the 2-MBI molecules. The initial presence of native copper oxides at the interface promotes the formation of Cu(I)-2-MBI metal …