Eco-friendly preparation of advanced epoxy composites and their pyrolysis and flame retardant mechanisms

Traditional additive flame retardants pose issues including high dosage, easy precipitation, and poor compatibility with the matrix. Designing efficient organic-inorganic synergistic flame retardants can enhance the flame retardancy and mechanical properties of epoxy (EP) composites while reducing their smoke toxicity. In our study, we initially employed Tetrakis(hydroxymethyl)phosphonium sulfate (THPS) for intercalation modification of montmorillonite (MMT). Subsequently, we achieved a green and efficient exfoliation of MMT by reacting urea with hydroxyl groups, resulting in the simultaneous preparation of efficient organic/inorganic synergistic flame retardants (THPSU-MMT). EP composites containing 5wt% THPSU-MMT can attain UL-94 V0 classification. Furthermore, the peak heat release rate (PHRR), total heat release (THR), and peak release rates of CO can be reduced by up to 78.42 %, 62.26 %, and 72.50 %, respectively. Simultaneously, we systematically investigated the synergistic flame retardant mechanism of the EP composite. The findings reveal that THPSU-MMT exhibits a dual flame retardant effect in both the gaseous and condensed phases. Moreover, the combination of MMT and THPSU substantially enhances the presence of phosphorus-containing pyrolysis products in the condensed phase. The fire performance index (FPI) of the flame retardant EP increased from 0.05 m2/s/W in pure EP to 0.36 m2/s/ W, attributed to the enhanced catalytic carbonization and assisted gas-phase free radical capture. Additionally, the flame spread index (FGI) decreased from 11.55 kW/m/s in pure EP to 1.18 kW/m/s, signifying a substantial enhancement in fire safety. Furthermore, the THPSU-MMT synergistic flame retardants improved the tensile strength of EP composites. This study offers an environmentally friendly and efficient approach for the effective exfoliation of MMT, while also presenting novel concepts for the design of efficient organic-inorganic synergistic flame retardants.