Amphiphilic Block Copolymers Directed Interface Coassembly to Construct Multifunctional Microspheres with Magnetic Core and Monolayer Mesoporous Aluminosilicate Shell

Abstract Core–shell magnetic porous microspheres have wide applications in drug delivery, catalysis and bioseparation, and so on. However, it is great challenge to controllably synthesize magnetic porous microspheres with uniform well‐aligned accessible large mesopores (>10 nm) which are highly desired for applications involving immobilization or adsorption of large guest molecules or nanoobjects. In this study, a facile and general amphiphilic block copolymer directed interfacial coassembly strategy is developed to synthesize core–shell magnetic mesoporous microspheres with a monolayer of mesoporous shell of different composition (FDUcs‐17D), such as core–shell magnetic mesoporous aluminosilicate (CS‐MMAS), silica (CS‐MMS), and zirconia‐silica (CS‐MMZS), open and large pores by employing polystyrene‐block‐poly (4‐vinylpyridine) (PS‐b‐P4VP) as an interface structure directing agent and aluminum acetylacetonate (Al(acac)₃), zirconium acetylacetonate, and tetraethyl orthosilicate as shell precursors. The obtained CS‐MMAS microspheres possess magnetic core, perpendicular mesopores (20–32 nm) in the shell, high surface area (244.7 m² g⁻¹), and abundant acid sites (0.44 mmol g⁻¹), and as a result, they exhibit superior performance in removal of organophosphorus pesticides (fenthion) with a fast adsorption dynamics and high adsorption capacity. CS‐MMAS microspheres loaded with Au nanoparticles (≈3.5 nm) behavior as a highly active heterogeneous nanocatalyst for N‐alkylation reaction for producing N‐phenylbenzylamine with a selectivity and yields of over 90% and good magnetic recyclability.