Catalyst-Free Oxidation of Styrene to Styrene Oxide Using Circulating Microdroplets in an Oxygen Atmosphere.

Abstract

Water microdroplets possess unique interfacial properties that enable chemical reactions to occur spontaneously and increase the reaction rate by orders of magnitude. In this study, water containing styrene (SY) was cyclically sprayed into the air to form microdroplets with an average diameter of 6.7 μm. These microdroplets allowed SY to be oxidized into styrene oxide (SO) without catalysts. No oxidation products of SY were observed in the bulk solution under the same conditions, while in microdroplet reactions 4.2% conversion of SY with approximately 3.1 mM SO was detected. Compared with the traditional spraying microdroplet method, the oxidation product concentration was enhanced by 1000 times. Experiments proved that an aerobic environment boosts SY oxidation, leading to a proposed dual-path hydrogen peroxide (H2O2) oxidation mechanism at the droplet interface. This was confirmed by density functional theory calculations (DFT). Furthermore, in the presence of additional ultrasound, the SY oxidation process initiated by water droplets can be further enhanced, and 7.0% conversion of SY with approximately 5.2 mM SO was detected. The cyclic spraying method greatly enhanced the oxidation product concentration, showing the potential for large scale chemical production using microdroplets.