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New poly(amide‐imide) Mg‐Al/layered double hydroxide (LDH) nanocomposites (PAINC) were prepared from synthesized poly(amide‐imide) (PAI) containing sulfone and ether linkages with two new organo modified Mg‐Al LDH (OLDH) by solution intercalation technique. OLDH were prepared from two different organo modifier with and without imide heterocyclic structure by one step method. The results of X‐ray diffraction (XRD), field emission‐scanning electron microscopy (FE‐SEM) and transmission electron microscopy (TEM) showed uniform distribution for LDH sheets in the PAI matrix. Thermal properties of all the samples were studied by thermogravimetric analysis (TGA) and differential scanning calorimetry (DSC). The thermal properties results showed that by OLDH loading in PAI matrix the thermal stabilities were increased. The temperature at 5% mass loss (T5) was increased from 225°C to 300°C for PAINC containing 5 mass% of OLDH containing imide hetrocyclic rings. The theoretical study indicated that the d‐value of OLDH has been related to structure of its organo‐modifier. POLYM. COMPOS., 39:E1669–E1681, 2018. © 2017 Society of Plastics Engineers

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