Tunable negative permittivity behavior and excellent electromagnetic shielding performance of pyrolytic carbon‐glass fiber felt/epoxy resin metacomposites

Abstract Effective and accurate adjustment of negative permittivity behavior is worthy of further investigation. Herein, pyrolytic carbon‐glass fiber felt/epoxy resin (PyC‐GFF/ER) metacomposites with tunable negative permittivity were prepared using an impregnation‐calcination method. The permittivity, electrical conductivity, and electromagnetic shielding performance of the polymer metacomposites were investigated. Due to the inherent three‐dimensional structural network of GFF, the PyC adhering to the surface of glass fiber easily formed a conductive network in the composites. As the PyC content increased in the ER composites, the conductivity mechanism changed from hopping conduction to metal‐like conduction. The ER composites with high PyC contents showed negative permittivity behavior and the epsilon‐near‐zero response owing to the low frequency plasma state of free electrons in the PyC‐conduction network. By controlling the PyC content, the negative permittivity behavior of ER composites could be effectively tuned. With the increase in PyC content, the values of negative permittivity increased, and the epsilon‐near‐zero frequency shifted to a higher frequency. Moreover, the ER composites with high PyC contents showed excellent electromagnetic shielding properties (29.4 dB) at X‐band. This work not only provided a feasible method to realize the tunable negative permittivity of polymer metacomposites, but also promoted its application in the microwave field. Highlights The pyrolytic carbon‐glass fiber felt/epoxy resin composites were fabricated. The negative permittivity was first reported in the PyC‐GFF/ER composites. Tunable negative permittivity could be well explained by Drude model. The polymer composites had excellent electromagnetic shielding property.