Binary layered double hydroxides (LDHs) of Mg-Al and Co-Al having varied cation molar ratio were studied for the catalytic epoxidation of styrene with molecular O(2) as an oxidant and DMF as a solvent. The effect of various reaction variables, reconstruction and reuse of LDH samples on the catalytic activity was evaluated. The cation molar ratio of LDH as well as concentration of DMF significantly affected the catalytic activity. The highest styrene conversion was observed with LDH having cation molar ratio (Mg/Co:Al) of 3:1. Mg-Al LDH showed highest styrene conversion of 85% with 80% styrene oxide selectivity and Co-Al LDH sample exhibited highest styrene conversion of 97% with 83% oxide selectivity at 100 degrees C after 4h. (C) 2011 Elsevier B.V. All rights reserved.