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Magnetic assembly at the nanoscale level brings potential possibilities in obtaining novel delicate nanostructures with unique physical, photonic or electronic properties. Interface surfactant micelle-directed assembly strategy holds great promising in fabricating ordered mesoporous materials with multifunctionality and pore parameter tunability. Combing these, herein, one-dimensional (1D) nanochains with well-aligned silica-coated magnetic particles as core and mesoporous aluminosilicate as shell are rational fabricated for the first time through magnetic field induced interface coassembly in biliquid system followed by the incorporation of Al species via in-situ chemical modification and transformation strategy. The obtained magnetic mesoporous aluminosilicate nanochains (MMAS-NCs) possess well-defined core–shell–shell sandwich nanostructure, tunable perpendicular mesopore channels in the shell (2.7–7.6 nm), high surface area (359 m2·g-1), abundant acidic sites, and superparamagnetism with a magnetization saturation of 13.8 emu·g-1. Thanks to the unique properties, the MMAS-NCs exhibit excellent performance in acting as magnetically recyclable superior solid acid catalysts and nanostirrers with high conversion of over 96.8%, selectivity of 95.0% in the deprotection reaction of benzaldehyde dimethylacetal to benzaldehyde. Moreover, MMAS-NCs exhibit an interesting pore size effect on the catalytic activity, namely, in the pore size range of 2–8 nm, the catalysts with larger pores show significantly enhanced catalytic activity due to the balanced mass transport and density of surface active sites.
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