Using Resonance-Enhanced Multiphoton Ionization Time-of-Flight Mass Spectrometry to Evaluate the Movement of a Constituent in a Multiple Emulsion

[Image: see text] Herein, we propose a method for evaluating the movement of a constituent in a multiple emulsion while maintaining its original dispersed condition. In this study, an oil-in-water-in-oil (O(1)/W/O(2)) emulsion was prepared using a two-step emulsification method with styrene as an analyte species in the inner phase (O(1)). The emulsion was measured using resonance-enhanced multiphoton ionization time-of-flight mass spectrometry without pretreatment such as centrifugation. From a series of obtained mass spectra, a time profile for the peak areas arising from styrene was constructed. When the emulsion was measured immediately following preparation, a time profile composed of a base, positive, and negative signals confirmed the presence of styrene in the O(2), O(1), and W phases, respectively. Moreover, while a small amount of styrene was present in the inner O(1) phase, almost all of the styrene was found in the outer O(2) phase. Furthermore, the results of the obtained time profile were converted into a box plot, and a method for the selection of the base, positive, and negative signals was tentatively determined. Then, the movement of styrene among the phases could be evaluated using the time courses of these signals; the time constant of the movement of styrene from an O(1)/W droplet to the O(2) phase was calculated to be 0.8 h.