One-Step Synthesis of Hydrophobic Multicompartment Organosilica Microspheres with Highly Interconnected Macro-mesopores for the Stabilization of Liquid Marbles with Excellent Catalysis

Abstract

The combination of an emulsion template with polymerization is a very convenient approach to the one-step realization of both simple control porous structures via a change in emulsion formulation and easy functionalization via the concomitant choice of an on-demand monomer. A major challenge of this approach is the inherent instability of the oil/water interface in emulsions, especially the occurrence of chemical reactions in oil or aqueous phases. This study reports the pioneering preparation of highly interconnected macro-mesopores and multicompartment (HIMC) vinyl organosilica microspheres with hydrophobicity by the one-step formation of W/O/W emulsions acting as a template. The emulsion system consists of acidified deionized water, a stabilizer, and vinyltriethoxysilane (VTEO) in which VTEO can be used to produce an organosilica skeleton of the resultant microsphere by a sol-gel process. The study demonstrated that the marvelous stability of W/O/W emulsions aids the formation of multicompartment organosilica microspheres with highly interconnected macro-mesopores by emulsion droplets rather than single-compartment (SC) microspheres. Meanwhile, the internal porous structure and surface morphology of as-prepared organosilica microspheres could be largely tuned by a simple variation of the pH value, the volume fraction of the water phase, and the stabilizer concentration in the initiating multiemulsions. Benefiting from such a well-orchestrated structure and the existence of numerous vinyl groups on the surface, HIMC organosilica microspheres exhibit very high hydrophobicity (with a water contact angle larger than 160°), which allows them to stabilize liquid marbles with excellent stability and high mechanical robustness. Because of its strong catalyst, Ag nanoparticles within HIMC organosilica microspheres enable Ag/HIMC-vinyl organosilica microsphere-based liquid marbles to be an efficient catalytic microreactor, realizing the complete degradation of MB to leuco methylene blue by NaBH₄ in 10 min. The result of this work could provide some guidance for the easy, low-cost, benign preparation of HIMC microspheres having the potential to be excellent supporter of metal nanoparticles or other functionalized compounds for applications in sensing, optoelectronics, and catalysis.