This work focuses on the preparation, characterization, and comparison of porous systems derived from three layered materials: Na-ilerite (an Al-free sodium silicate), bentonite (a clay mineral), and MWW-precursor (a layered zeolite). Two post-synthetic modifications were employed: swelling/pillaring and swelling/delamination, to assess their effects on the textural properties and catalytic activity in NH3-SCR. The swelling/pillaring method yielded porous structures with greater surface area and pore volume than the swelling/delamination approach. Notably, the microporous surface area of SiO2-pillared ilerite increased dramatically from 0.16 m²/g to 898 m²/g. For MWW, swelling/delamination resulted in a porous system with a significant mesoporous volume (1.26 cm³/g), contrasting with the purely microporous parent MWW-precursor. In NH3-SCR applications, Fe-containing SiO2-pillared MWW and delaminated MWW catalysts exhibited the highest catalytic activity, achieving 57% and 48% NOx reduction at 500 °C, respectively. Despite the lower BET surface area of these catalysts compared to SiO2-pillared ilerite, the latter's Al-free composition was a critical factor. When aluminum was incorporated, the catalytic activity of ilerite improved, reaching 56% in the Al2O3-pillared variant.
