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Relaxations and relaxor-ferroelectric-like response of nanotubularly confined poly(vinylidene fluoride)

AuthorsMartín, Jaime; Iturrospe, Amaia; Cavallaro, Andrea ; Arbe, Arantxa ; Stingelin, Natalie; Ezquerra, Tiberio A. ; Mijangos, Carmen ; Nogales, Aurora
Issue Date19-Mar-2017
PublisherAmerican Chemical Society
CitationChemistry of Materials 29(8): 3515-3525 (2017)
AbstractHerein, we elucidate the impact of tubular confinement on the structure and relaxation behavior of poly(vinylidene difluoride) (PVDF) and how these affect the para-/ferroelectric behavior of this polymer. We use PVDF nanotubes that were solidified in anodic aluminum oxide (AAO) templates. Dielectric spectroscopy measurements evidence a bimodal relaxation process for PVDF nanotubes: besides the bulk-like α-relaxation, we detect a notably slower relaxation that is associated with the PVDF regions of restricted dynamics at the interface with the AAO pore. Strikingly, both the bulk-like and the interfacial relaxation tend to become temperature independent as the temperature increases, a behavior that has been observed before in inorganic relaxor ferroelectrics. In line with this, we observe that the real part of the dielectric permittivity of the PVDF nanotubes exhibits a broad maximum when plotted against the temperature, which is, again, a typical feature of relaxor ferroelectrics. As such, we propose that, in nanotubular PVDF, ferroelectric-like nanodomains are formed in the amorphous phase regions adjacent to the AAO interface. These ferroelectric nanodomains may result from an anisotropic chain conformation and a preferred orientation of local dipoles due to selective H-bond formation between the PVDF macromolecues and the AAO walls. Such relaxor-ferroelectric-like behavior has not been observed for nonirradiated PVDF homopolymer; our findings thus may enable in the future alternative applications for this bulk commodity plastic, e.g., for the production of electrocaloric devices for solid-state refrigeration which benefit from a relaxor-ferroelectric-like response.
Publisher version (URL)http://doi.org/10.1021/acs.chemmater.6b05391
Identifiersdoi: 10.1021/acs.chemmater.6b05391
issn: 1520-5002
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