There is renewed interest in studying chemical reactions of surfactant molecules in monolayer arrays at the air-water interface. High-performance liquid chromatography and vapor-phase chromatography have been used for the first time to detect, quantitate, and help characterize the small amounts of material contained in such surface films, ca. 10-9-10-10 mol/cm2. A multicompartment trough has been designed and used to allow a series of chemical reactions to be performed upon a welldefined monolayer film. The alkaline hydrolysis of |(bpy)2Ru11[bpy(COOR)2]|2+ in monolayer films (R = C18H37) is found to proceed more rapidly than in homogeneous, aqueous solution (R = C2H5) at the same bulk pH. Monitoring the stability of surface films and their hydrolytic reactions by chromatography has proven superior to observing area changes at constant surface pressure. © 1979, American Chemical Society. All rights reserved.