A modular approach for the design of two-component supramolecular polymer (SMP) networks is reported. A series of materials was prepared by blending two (macro)monomers based on trifunctional poly(propylene oxide) (PPO) cores that were end-functionalized with hydrogen-bonding 2-ureido-4[1H]pyrimidinone (UPy) groups. One monomer was based on a PPO core with a number-average molecular weight (M_n) of 440 g mol^–1. The SMP formed by this building block is a glassy, brittle material with a glass transition temperature (T_g) of about 86 °C. The second monomer featured a PPO core with an M_n of 3000 g mol^–1. The SMP formed by this building block adopts a microphase-segregated morphology that features a rubbery phase with a T_g of −58 °C and crystalline domains formed by the UPy assemblies, which act as physical cross-links and melt around 90–130 °C. Combining the two components allows access to microphase-segregated blends comprised of a rubbery phase constituted by the high-M_n cores, a glassy phase formed by the low-M_n component, and a crystalline phase formed by UPy groups. This allowed tailoring of the mechanical properties and afforded materials with storage moduli of 37–609 MPa, tensile strengths of 2.0–5.4 MPa, and melt viscosities of as low as 11 Pa s at 140 °C. The materials can be used as reversible adhesives.

中文翻译：

---

玻璃状超分子聚合物网络的增韧

报告了一种用于设计双组分超分子聚合物 (SMP) 网络的模块化方法。通过混合两种基于三官能聚（环氧丙烷）（PPO）核的（大）单体制备了一系列材料，这些核用氢键 2-ureido-4[ 1H ]嘧啶酮（UPy）基团进行了末端功能化。一种单体基于数均分子量 ( _Mn )为 440 g mol ^–1的 PPO 核。由这种结构单元形成的 SMP 是一种玻璃状、脆性材料，玻璃化转变温度 ( Tg ) 约为 86 °C _。第二个单体的特点是 PPO 核心，Mn_为3000 g mol ^–1. 由这种结构单元形成的 SMP 采用微相分离形态，其特征在于T _g为 -58°C的橡胶相和由 UPy 组件形成的结晶域，它们充当物理交联并在 90-130° 左右熔化C。将这两种组分结合可以得到微相分离的共混物，该混合物包括由高Mn核心构成的橡胶相、由低Mn 组分形成的玻璃相_和由UPy基团形成的结晶相。这允许定制机械性能并提供具有 37-609 MPa 的储能模量、2.0-5.4 MPa 的拉伸强度和在 140°C 下熔体粘度低至 11 Pa s 的材料。该材料可用作可逆粘合剂。