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Novel bifunctional acid–base monolayered hybrid catalysts (MLHMs), based on associated individual (organo)aluminosilicate sheets with amino and sulfonic pending groups located in the interlayer space, have been successfully prepared by direct alkaline hydrothermal synthesis and evaluated in consecutive catalytic transformations. Different characterization techniques such as chemical and thermogravimetrical analyses, X-ray diffraction, TEM microscopy, nuclear magnetic resonance (NMR), temperature-programmed desorption of CO2 and NH3 (TPD), and textural measurements were used to show the physicochemical and structural nature of the materials, evidencing their effectiveness as functional acid, base, and acid–base catalysts for different one-pot two-step tandem reactions, which were performed in the presence of only one active and recoverable lamellar-type hybrid solid catalyst.

Functional Acid and Base Hybrid Catalysts Organized by Associated (Organo)aluminosilicate Layers for C–C Bond Forming Reactions and Tandem Processes