Flexible and highly filled conductive polymer composites with strong mechanical properties are highly desirable as electromagnetic interference (EMI) shielding and thermally conductive materials for human protection and wearable devices. Herein, a tough interface has been built up by the combination of polydopamine modification and pH triggered hydrogen bonding to prepare flexible and mechanically robust waterborne polyacrylate/graphene@polydopamine composites. Graphene was modified with polydopamine via an in-situ polymerization method. By adjusting the initial pH value in the film formation process, the transition from electrostatic repulsion to hydrogen bonding between graphene@polydopamine and polyacrylate was engineered for improving the mechanical properties. At optimal pH value, the maximum tensile strength of the composite is enhanced by 137% compared with that of neat polymer matrix. Moreover, the composite with filler loading of 20 wt% exhibits an EMI shielding effectiveness of 58 dB at 0.6 mm thickness and thermal conductivity of 1.68 W/m·K, respectively. The practical application of the composite film and composite coated leather also demonstrates their outstanding flexibility, EMI shielding, and heat dissipation performance, indicating their excellent potential as EMI shielding and thermally conductive materials in wide areas such as wearable devices, telecommunication systems, and human protection.

具有强机械性能的挠性且高度填充的导电聚合物复合材料非常理想，可作为电磁干扰（EMI）屏蔽材料和用于人体保护和可穿戴设备的导热材料。在此，通过聚多巴胺改性和pH触发的氢键结合，已经建立了坚韧的界面，以制备柔性的和机械坚固的水性聚丙烯酸酯/石墨烯@聚多巴胺复合材料。石墨烯通过原位聚合方法用聚多巴胺改性。通过调节成膜过程中的初始pH值，设计了石墨烯@聚多巴胺和聚丙烯酸酯之间从静电排斥到氢键的过渡，以改善机械性能。在最佳pH值下，与纯聚合物基体相比，复合材料的最大拉伸强度提高了137％。此外，填料含量为20 wt％的复合材料在0.6 mm厚度下的EMI屏蔽效率为58 dB，热导率分别为1.68 W / m·K。复合膜和复合涂层皮革的实际应用还展示了其出色的柔韧性，EMI屏蔽和散热性能，表明它们在广泛的领域（如可穿戴设备，电信系统和人员防护）中具有作为EMI屏蔽和导热材料的出色潜力。 。分别。复合膜和复合涂层皮革的实际应用还展示了其出色的柔韧性，EMI屏蔽和散热性能，表明它们在广泛的领域（如可穿戴设备，电信系统和人员防护）中具有作为EMI屏蔽和导热材料的出色潜力。 。分别。复合膜和复合涂层皮革的实际应用还展示了其出色的柔韧性，EMI屏蔽和散热性能，表明它们在广泛的领域（如可穿戴设备，电信系统和人员防护）中具有作为EMI屏蔽和导热材料的出色潜力。 。