In this work, a hydrosoluble matrix is used for the first time to prepare flexible membranous composites, in order to improve their environmental friendliness and simplify the processing. Modified graphene (GR) sheets are distributed in polyvinyl alcohol (PVA) solution to achieve flexible GR/PVA metacomposites. As graphene content increases, an interconnected graphene network is eventually formed among the PVA matrix, and the resulting composites present a conductor‐like behavior. Interestingly, the Drude‐like negative permittivity is obtained in the composites with 20 wt% graphene, which is ascribed to the plasma oscillation. Meanwhile, the absolute values of negative permittivity decrease by several orders of magnitude due to the moderate electron density of graphene. It is demonstrated that the negative permittivity is dependent on the inductive character. This work provides a novel and versatile approach based on water‐soluble matrices to prepare flexible membranous metacomposites, which can be applied in wearable cloaking, thin‐film capacitors, and flexible and stretchable devices.

中文翻译：

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具有负介电常数行为的水溶性石墨烯/聚乙烯醇膜状复合材料

在这项工作中，首次使用水溶性基质来制备柔性膜状复合材料，以提高其环境友好性并简化加工过程。改性石墨烯（GR）片材分布在聚乙烯醇（PVA）溶液中，以实现灵活的GR / PVA元复合材料。随着石墨烯含量的增加，最终在PVA基质之间形成了相互连接的石墨烯网络，所得复合材料表现出类似导体的行为。有趣的是，在具有20 wt％石墨烯的复合材料中获得了类似Drude的负介电常数，这归因于等离子体振荡。同时，由于石墨烯的中等电子密度，负介电常数的绝对值降低了几个数量级。已经证明负介电常数取决于感应特性。这项工作提供了一种基于水溶性基质的新颖而通用的方法来制备柔性膜状超复合材料，该方法可用于可穿戴隐身衣，薄膜电容器以及柔性和可拉伸设备中。