Negative Capacitance in Nanocomposite Based on High-Density Polyethylene (HDPE) with Multiwalled Carbon Nanotubes (CNTs).

Negative capacitance (NC), already observed in conducting polymer-based nanocomposites, was recently reported and evidenced at low frequencies (<10 kHz) in non-conducting polymer-based nanocomposites containing conductive particles. In this contribution, we demonstrate that it is possible to produce economic high-density polyethylene (HDPE) nanocomposites exhibiting an NC effect at low frequencies via a convenient and environmentally friendly extrusion-like process by only adjusting the duration of melt-mixing. Nanocomposite materials are produced by confining a limited quantity, i.e., 4.6 wt.%, of multiwalled carbon nanotubes (CNTs) within semi-crystalline HDPE to reach the percolation threshold. With increasing melt processing time, crystallites of HDPE developing at the surface of CNTs become bigger and perturbate the connections between CNTs leading to a dramatic change in the electrical behavior of the systems. More specifically, the link between NC and current oscillations is stressed while the dependence of NC with the size of polymer crystallites is evidenced. NC tends to appear when space charge effects take place in HDPE/MWCNT interfaces, in structures with convenient crystallite sizes corresponding to 10 min of melt-mixing.