Non-isocyanate poly(urethane)s (NIPU)s have emerged as an environmentally friendly alternative for conventional polyurethanes, but several challenges remain towards their wide-scale adoption (e.g., attainment of high molecular weights for sufficiently effective mechanical properties and ease of application). Adopting NIPUs as hybrid polymer-polymer particles with methacrylic monomers is one route towards obtaining higher overall molecular weight, improving properties, and introducing advantages of methacrylate functionality. First, NIPU latex was synthesized using dicarbonate terminated poly (propylene glycol) and the commercial vegetable oil-based diamine Priamine 1075 via step miniemulsion polymerization yielding stable particles with sizes <220 nm. Then, the NIPU latex was used as the seed for the synthesis of hybrid NIPU-poly(methacrylate) particles via conventional radical emulsion statistical copolymerization of a long side chain (13 alkyl groups) alkyl methacrylate (C13MA) and isobornyl methacrylate (IBOMA). Two polymeric phases were observed in cryo-microtomed TEM of the dried latexes at ambient temperature, indicating core-shell phase-separated morphologies. Moreover, 2-acetoacetoxyethyl methacrylate (AAEMA) was introduced in the formulation containing the methacrylate phase to impart dynamic covalent crosslinking into the hybrid via ketone-amine vinylogous urethane formation, resulting in materials with stress relaxation up to 90% at 130 °C and one-time recycled films with similar stress-strain profiles as the original films.

非异氰酸酯聚氨基甲酸酯 (NIPU) 已成为传统聚氨酯的环保替代品，但其大规模采用仍面临一些挑战（例如，获得高分子量以获得足够有效的机械性能和易于应用） ）。采用 NIPU 作为具有甲基丙烯酸单体的杂化聚合物-聚合物颗粒是获得更高总分子量、改善性能和引入甲基丙烯酸酯官能团优势的一种途径。首先，使用二碳酸酯封端的聚丙二醇和商用植物油基二胺Priamine 1075，通过分步细乳液聚合合成NIPU乳胶，产生尺寸<220 nm的稳定颗粒。然后，以NIPU乳胶为种子，通过长侧链（13个烷基）甲基丙烯酸烷基酯（C13MA）和甲基丙烯酸异冰片酯（IBOMA）的常规自由基乳液统计共聚合成杂化NIPU-聚（甲基丙烯酸酯）颗粒。在环境温度下干燥乳胶的冷冻显微切片 TEM 中观察到两个聚合物相，表明核-壳相分离的形态。此外，在含有甲基丙烯酸酯相的配方中引入了甲基丙烯酸 2-乙酰乙酰氧基乙酯 (AAEMA)，通过酮-胺插烯氨基甲酸酯的形成赋予杂化物动态共价交联，从而使材料在 130 °C 下应力松弛高达 90%，并且- 具有与原始薄膜相似的应力应变曲线的时间再生薄膜。