LAUSR

Abstract Metacomposites with conductive polymer matrix toward negative permittivity have promising applications in energy storage devices and electromagnetic shielding. In this paper, carbon nanotubes (CNTs)/polypyrrole (PPy) nanocomposites with different loadings of CNTs have been synthesized using a surface-initiated polymerization (SIP) method. Scanning electron microscopy (SEM) results indicate that conductive networks have constructed inside the nanocomposites by CNTs and PPy granules. A frequency switch of permittivity from positive to negative in pure PPy and CNTs/PPy nanocomposites with low CNTs loading (1 wt%) is observed, which can be analyzed by the Lorentz model. Besides, all negative permittivity behavior in the test frequency range (10–1000 MHz) is found in CNTs/PPy nanocomposites with higher CNTs content which can be easily tuned by adjusting the CNTs loading. Negative permittivity is considered arising from the plasma oscillation of delocalized electrons in conductive networks and could be fitted by Drude model. Furthermore, the equivalent circuit models, ac conductivity and dielectric loss are discussed.