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Smart Pickering Emulsions Co-Stabilized by Chalcogenoviologen Surfactants and Single-Atom Pt-Decorated g-C3N4 for
Zhaohui Cui1, Siyu Sun1, Tianyue Yuan1
1Frontier Institute of Science and Technology, Interdisciplinary Research Center of Frontier Science and Technology, State Key Laboratory for Strength and Vibration of Mechanical Structures, Institute of New Concept Sensors and Molecular Materials, Shaanxi Key Laboratory of New Conceptual Sensors and Molecular Materials, Engineering Research Center of Key Materials for Efficient Utilization of Clean Energy of Shaanxi Province, National innovation Platform (Center) for Industry-Education Integration of Energy Storage Technology, Xi'an Key Laboratory of Electronic Devices and Material Chemistry, School of Physics, Xi'an Jiaotong University, Xi'an, Shaanxi Province710054, China.
Abstract:
Interfacial reaction microenvironments play a critical role in determining photocatalytic performance beyond the intrinsic properties of photocatalysts. However, emulsion-based photocatalytic platforms that simultaneously offer structural robustness, switchable operation, and efficient interfacial charge-transfer regulation remain rare. Herein, smart-responsive Pickering emulsions are developed by costabilization of chalcogenoviologen surfactants (SV2+-UDA/SeV2+-UDA/TeV2+-UDA) and single-atom platinum-decorated graphitic carbon nitride (Pt SAs@g-C3N4) for biphasic photocatalysis. The resulting emulsions exhibit outstanding stability in strong acidic and alkaline media as well as in saturated brine while allowing reversible demulsification and re-emulsification under an external electric field, thereby enabling switchable catalysis and catalyst recovery. The optimized emulsion achieves a hydrogen evolution rate of up to 7824 μmol·h-1·g-1 under visible-light irradiation, corresponding to a 3.0-fold enhancement over the bulk aqueous, viologen-free system, while retaining over 90% of its activity across a wide pH range and under seawater salinity. More importantly, the emulsion functions as a bidirectional microreactor, coupling aqueous hydrogen evolution with oil-phase oxidative coupling of benzylamine without sacrificial reagents, and delivers imine yields above 85% together with a hydrogen evolution rate of 3892 μmol·h-1·g-1. The enhanced performance highlights the critical role of interfacial synergy. The surfactant/photocatalyst costabilization strategy provides a versatile platform for robust, switchable, and synergistic biphasic photocatalysis.
