Multi-wall carbon nanotubes (MWCNTs), graphene nanoplates (GNPs), and hybrid fillers (MWCNTs/GNPs) filled thermoplastic polyurethane (TPU) nanocomposites are prepared via melt mixing. The effects of the fillers (contents of 1, 2, and 3 wt%), shear rate, and temperature are investigated on the rheological behavior of the TPU nanocomposites. The results demonstrate that the TPU/MWCNT nanocomposites exhibit stronger polymer-filler and filler-filler interactions than the TPU/GNP and TPU/GNP/MWCNT nanocomposites, and the interactions are destroyed at higher shear rates. Anomalous rheological behavior is found in the nanocomposites with 2 and 3 wt% MWCNTs (2CNT and 3CNT) and 3 wt% MWCNTs/GNPs (3Hybrid). Specifically, as rising the temperature at higher temperatures (180–190 °C), the melt complex viscosities in the low frequency region (<0.4 rad/s) are slightly increased for the 2CNT and 3Hybrid samples, and are more increased over a broader frequency region (<10 rad/s) for the 3CNT sample. The Fourier transform infrared spectroscopy spectra demonstrate that the anomalous rheological behavior is not caused by hydrogen bonding in the TPU nanocomposites. The anomalous rheological behavior is revealed to be attributed to the fact that stronger polymer-filler and filler-filler interactions exist in the 2CNT, 3Hybrid and especially 3CNT samples, and the interactions are strengthened with rising temperature at higher temperatures. • Effect of different fillers on rheological behavior of TPU nanocomposites was investigated. • Anomalous viscosity increase with rising temperature for TPU nanocomposites was observed. • Mechanism behind anomalous rheological behavior was explored. • Stronger polymer-filler and filler-filler interactions resulted in anomalous rheological behavior.
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