Synergistic Effect of Multifunctional Layered Double Hydroxide-Based Hybrids and Modified Phosphagen with an Active Amino Group for Enhancing the Smoke Suppression and Flame Retardancy of Epoxy

To improve the fire hazard of epoxy resin (EP), phosphomolybdate (PMoA), as a classical Keggin cluster, was successfully intercalated into Mg, Al, and Zn layered double hydrotalcite (LDH) by the reconstruction method, and it was denoted as MgAlZn-LDH-PMoA. The structure and morphology of MgAlZn-LDH-PMoA were characterized by X-ray diffraction and Fourier transform infrared spectroscopy. Subsequently, hexa(4-aminophenoxy)cyclotriphosphazene (HACP) was prepared and characterized as a high-performance organic flame retardant, which is rich in flame elements phosphorus and nitrogen. The synergistic effects of MgAlZn-LDH-PMoA and HACP on the fire safety of EP composites loaded with different amounts of flame retardant hybrids were studied in detail. Thermogravimetric analysis showed that the char residue of these EP composites increased significantly. Compared with the EP matrix filled with only MgAlZn-LDH-PMoA or HACP, the incorporation of MgAlZn-LDH-PMoA and HACP had a synergistic effect on promoting char formation of EP composites. Particularly, the char yield of EP7 is as high as 29.0%. Furthermore, the synergistic effects of incorporation of MgAlZn-LDH-PMoA with HACP were investigated using the cone calorimeter combustion tests. The results showed that the total heat release and peak heat release rate of the EP composites remarkably declined by 35.2 and 50.9%, respectively, with a loading of 7 wt % hybrid flame retardant. Moreover, the hybrid flame retardants also showed an obvious inhibitory effect on the total smoke production and the release of toxic CO gas. The detailed analysis of the residual char indicated that the main mechanism for improving the flame retardancy and smoke suppression performance is due to both the catalytic carbonization of MgAlZn-LDH-PMoA and phosphoric acid compounds and physical barrier function of the char layer. In addition, the molybdenum oxides produced from [PMo12O40]3– during combustion can not only increase the yield and compactness of the char layer but also reduce the release of CO through a redox reaction, which has important application value to reduce the fire hazard.