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The layered double hydroxides (LDH) of Mg2AlNi and Mg3Al pillared by Keggin-type phosphotungstic acid anion (POM), i.e. Mg2AlNi-POM LDH and Mg3Al-POM LDH were synthesized by an ion-exchange method. The synthesized POM intercalated LDH compounds were characterized using various techniques such as FTIR, XRD, TGA and BET. The observed results show that the obtained catalysts retain the layer structure of LDH. Compared with the binary Mg3Al-POM LDH, the ternary Mg2AlNi-POM LDH catalyst indicated a higher thermal and chemical stability. The catalytic activity of the resulting LDH-POM was also assessed in the green oxidation of cyclohexanol with aqueous H2O2 as an oxidant. The Mg2AlNi-POM LDH showed a much higher conversion and selectivity for cyclohexanone than the corresponding Mg3Al-POM LDH catalyst.