Developing polymers with both flame-retardant and smoke-suppressing properties is a great challenge in the field of fire-safety thermoplastic polyurethane (TPU). This study involved synthesizing a synergistic organic-hybrid layered double hydroxide (O-LDH) and phosphorus/nitrogen-containing substance (PD) inspired by the observed synergistic effect between them. The incorporation of PD significantly enhanced the flame-retardant properties of TPU in conjunction with cobalt/aluminum- layered double hydroxide. The composite containing 10 wt% O-LDH achieved a limiting oxygen index of 26.5% and met the vertical burning V-0 rating. Moreover, the heat and smoke release were decreased compared to pure TPU in cone calorimeter tests. The systematic characterization of the synergistic flame-retardant mechanism emphasized the crucial contribution of cobalt and phosphorus species in catalyzing charring effects, resulting in the compact and highly carbonized char layer in the condensed phase. The incorporation of the hybrid flame retardant significantly enhanced the advancement of the flame-retardant TPU materials.
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