One of the current challenges in the development of flame retardants is the preparation of an environmentally friendly multi-element synergistic flame retardant to improve the flame retardancy, mechanical performance, and thermal performance of composites. This study synthesized an organic flame retardant (APH) using (3-aminopropyl) triethoxysilane (KH-550), 1,4-phthalaadehyde, 1,5-diaminonaphthalene, and 9,10-dihydro-9-oxa-10-phosphaphenanthrene-10-oxide (DOPO) as raw materials, through the Kabachnik-Fields reaction. Adding APH to epoxy resin (EP) composites could greatly improve their flame retardancy. For instance, UL-94 with 4 wt% APH/EP reached the V-0 rating and had an LOI as high as 31.2%. Additionally, the peak heat release rate (PHRR), average heat release rate (AvHRR), total heat release (THR), and total smoke produced (TSP) of 4% APH/EP were 34.1%, 31.8%, 15.2%, and 38.4% lower than EP, respectively. The addition of APH improved the mechanical performance and thermal performance of the composites. After adding 1% APH, the impact strength increased by 15.0%, which was attributed to the good compatibility between APH and EP. The TG and DSC analyses revealed that the APH/EP composites that incorporated rigid naphthalene ring groups had higher glass transition temperatures (Tg) and a higher amount of char residue (C700). The pyrolysis products of APH/EP were systematically investigated, and the results revealed that flame retardancy of APH was realized by the condensed-phase mechanism. APH has good compatibility with EP, excellent thermal performance, enhanced mechanical performance and rational flame retardancy, and the combustion products of the as-prepared composites complied with the green and environmental protection standards which are also broadly applied in industry.

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Enhancing the flame retardancy with minimal impact on the mechanical and thermal performances of polymers remains a challenge. This study synthesized a phosphorus/nitrogen‐containing silane compound (D) using polyformaldehyde, KH‐550, and 9,10‐dihydro‐9‐oxa‐10‐phosphaphenanthrene‐10‐oxide (DOPO) as raw materials through the Kabachnik‐Fields reaction. After that, D was grafted onto the surface of graphene after hydrothermal treatment to obtain a nano hybrid flame retardant (D‐GR). And D‐GR/EP composites exhibited good flame resistance (LOI = 30.1% and UL‐94 reaches the V‐1 rating) even if the load on D‐GR was 1 wt%. Indeed, the total heat release, the peak heat release rate (PHRR), and the total smoke release of 1% D‐GR/EP dropped by 13.54%, 28.62%, and 44.32%, respectively, in comparison to pure EP. The mechanical performance of 1% D‐GR/EP was effectively maintained, as indicated by the results of impact, tensile and flexural tests. A systematic evaluation indicated that the accession of D‐GR effectively inhibited smoke and heat releases that are ascribed to the synergistic effect of phosphorus/nitrogen‐containing silane compound and graphene. In this study, a facile method was provided for the synthesis of halogen‐free flame‐retardant epoxy composites with superior performances. The combustion products of the as‐prepared composites complied with green and environmental protection standards.