Aiming to impart epoxy with a phosphorous-free super-efficient fire safety and multifunctions via a facile interface-manipulation protocol, we innovatively proposed a proof of concept of a two-in-one catalytic function via covalently inducing an interfacial supramolecular assembly of Salen-Fe complex on organic layered double hydroxide (LDH-DBS). Various characterizations confirmed the target LDH-DBS@Salen-Fe with a surface-located uniform and ultrathin deposition of Salen-Fe complex, which was conducive to a better nanodispersion in epoxy matrix. An exceptionally low loading of 2 wt% LDH-DBS@Salen-Fe (i.e., 0.6 % Salen-Fe) endowed epoxy with a UL-94 V-0 level and intensive fire protection with a suppressed peak heat release rate by 45.0 %. An insightful mechanism investigation demonstrated that the interface-located Salen-Fe rapidly catalyzed a charring reaction with an ultrafast formation of protective fire chars to resist an early-stage fire attack. Additionally, relative to EP/2LDH-DBS, a mere 0.6 % Salen-Fe increased the tensile, flexural and impact strength by 39.6 %, 31.5 % and 37.0 %, respectively based on the optimized interface compatibilization. Interestingly, an ultralow loading of Salen-Fe significantly contributed to a degradation recycling of epoxy under a mild condition with mass loss after 7 h treatment 392.8 % higher than its counterpart via catalytically promoting the generation of CHCOO∙ and HO∙ at the interface. In perspective, an interfacial supramolecular assembly of two-in-one catalysts exploits a novel route towards a phosphorous-free fire-safe and multifunctionally reinforced polymers.
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