The new sulfonic-acid-based Ce-Mn-Layered Doble Hydroxide (Ce-Mn-LDH@ CPTMS @NAP@SO3H) was prepared by modification of the Ce-Mn-layered double hydroxide (Ce-Mn-LDH) with 3-chloropropyltrimethoxysilane and N-amino phthalimide and functionalized with chlorosulfonic acid. Then, it was characterized with the FT-IR, XRD, EDX, SEM, SEM-mapping, UV/vis, TEM, and TGA-DTA techniques and used as a new and efficient heterogeneous acid catalyst for the green solvent-free synthesis of spiro[induline-pyran]ones and spiro[acenaphthylene-pyran] ones from the one-pot multicomponent condensation reaction of isatin or acenaphthoquinone, malononitrile, and 1,3-diketone in very short reaction times and excellent yields. Also, the catalyst is stable under reaction conditions and can be reused without the significant loss of catalytic activity.
