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In contrast to molecular-dipole polymers, such as PVDF, ferroelectrets are a new class of flexible spatially heterogeneous piezoelectric polymers with dosed or open voids that act as deformable macro-dipoles after charging.
With a spectrum of manufacturing processes being developed to engineer the heterogeneous structures, ferroelectrets are made with attractive piezoelectric properties well-suited for applications, such as pressure sensors, acoustic transducers, etc.
However, the sources of the macro-dipole charges have usually been the same, microscopic dielectric barrier discharges within the voids, induced when the ferroelectrets are poled under a large electric field typically via a so-called corona poling, resulting in the separation and trapping of opposite charges into the interior walls of the voids.
Such a process is inherently self-limiting, as the reverse internal field from the macro-dipoles eventually extinguishes the microdischarges, resulting in limited density of ions and not too high overall piezoelectric performance. Here, a new method to form ferroelectrets with gigantic electroactivity is proposed and demonstrated with the aid of an external ion booster.
A laminate consisting of expanded polytetrafluoroethylene (ePTFE) and fluorinated-ethylene-propylene (FEP) was prefilled with bipolar ions produced externally by an ionizer and sequentially poled to force the separation of positive and negative ions into the open fibrous structure, rendering an impressive piezoelectric d(33)( )coefficient of 1600 pC/N-an improvement by a factor of 4 in comparison with the d(33) of a similar sandwich poled with nonenhanced corona poling.
The (pre)filling dearly increases the ion density in the open voids significantly. The charges stored in the open-cell structure stays at a high level for at least 4 months. In addition, an all-organic nanogenerator was made from an ePTFE-based ferroelectret, with conducting poly(3,4-ethylene dioxythiophene): poly(styrenesulfonate) (PEDOT: PSS) coated fabric electrodes.
When poled with this ion-boosting process, it yielded an output power twice that of a similar sample poled in a conventional corona-only process. The doubling in output power is mainly brought about by the significantly higher charge density achieved with the aid of external booster.
Furthermore, aside from the bipolar ions, extra monopolar ions can during the corona poling be blown into the open pores by using for instance a negative ionic hair dryer to produce a unipolar ePTFE-based ferroelectret with its d(33) coefficient enhanced by a factor of 3. Ion-boosting poling thus unleashes a new route to produce bipolar or unipolar open-cell ferroelectrets with highly enhanced piezoelectric response.
The addition of nano-Al2O3 has been shown to enhance the breakdown voltage of epoxy resin, but its flashover results appeared with disputation. This work concentrates on the surface charge variation and dc flashover performance of epoxy resin with nano-Al2O3 doping. The dispersion of nano-Al2O3 in epoxy is characterized by scanning electron microscopy (SEM) and atomic force microscopy (AFM). The dc flashover voltages of samples under either positive or negative polarity are measured with a finger-electrode system, and the surface charge variations before and after flashovers were identified from the surface potential mapping. The results evidence that nano-Al2O3 would lead to a 16.9% voltage drop for the negative flashovers and a 6.8% drop for positive cases. It is found that one-time flashover clears most of the accumulated surface charges, regardless of positive or negative. As a result, the ground electrode is neighbored by an equipotential zone enclosed with low-density heterocharges. The equipotential zone tends to be broadened after 20 flashovers. The nano-Al2O3 is noticed as beneficial to downsize the equipotential zone due to its capability on charge migration, which is reasonable to maintain flashover voltage at a high level after multiple flashovers. Hence, nano-Al2O3 plays a significant role in improving epoxy with high resistance to multiple flashovers.
Non-linear dielectric spectroscopy (NLDS) is employed as an effective tool to study relaxation processes and phase transitions of a poly(vinylidenefluoride-trifluoroethylene-chlorofluoroethylene) (P(VDF-TrFE-CFE)) relaxor-ferroelectric (R-F) terpolymer in detail. Measurements of the non-linear dielectric permittivity epsilon 2 ' reveal peaks at 30 and 80 degrees C that cannot be identified in conventional dielectric spectroscopy. By combining the results from NLDS experiments with those from other techniques such as thermally stimulated depolarization and dielectric-hysteresis studies, it is possible to explain the processes behind the additional peaks. The former peak, which is associated with the mid-temperature transition, is found in all other vinylidene fluoride-based polymers and may help to understand the non-zero epsilon 2 ' values that are detected on the paraelectric phase of the terpolymer. The latter peak can also be observed during cooling of P(VDF-TrFE) copolymer samples at 100 degrees C and is due to conduction and space-charge polarization as a result of the accumulation of real charges at the electrode-sample interface.
The scientific career and the research activities of Paul Boening, especially during his tenures at Tongji University in Shanghai (Woosung Campus, 1922-1936) and the Technical University of Wroclaw (TH Breslau, 1936-1945), are briefly reviewed. In particular, Boening's pioneering investigations in the area of electrets and space charge in dielectrics are emphasized. We attempt to shed some light on the significant achievements of a virtually unknown contributor to the early history of electrets and of space-charge research and high-voltage engineering, during the 1920s and 1930s. It should be noted that dielectrics research was a truly international endeavor already at that time.
Due to their electrically polarized air-filled internal pores, optimized ferroelectrets exhibit a remarkable piezoelectric response, making them suitable for energy harvesting. Expanded polytetrafluoroethylene (ePTFE) ferroelectret films are laminated with two fluorinated-ethylene-propylene (FEP) copolymer films and internally polarized by corona discharge. Poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS)-coated spandex fabric is employed for the electrodes to assemble an all-organic ferroelectret nanogenerator (FENG). The outer electret-plus-electrode double layers form active device layers with deformable electric dipoles that strongly contribute to the overall piezoelectric response in the proposed concept of wearable nanogenerators. Thus, the FENG with spandex electrodes generates a short-circuit current which is twice as high as that with aluminum electrodes. The stacking sequence spandex/FEP/ePTFE/FEP/ePTFE/FEP/spandex with an average pore size of 3 mu m in the ePTFE films yields the best overall performance, which is also demonstrated by the displacement-versus-electric-field loop results. The all-organic FENGs are stable up to 90 degrees C and still perform well 9 months after being polarized. An optimized FENG makes three light emitting diodes (LEDs) blink twice with the energy generated during a single footstep. The new all-organic FENG can thus continuously power wearable electronic devices and is easily integrated, for example, with clothing, other textiles, or shoe insoles.
In our fast-changing world, human-machine interfaces (HMIs) are of ever-increasing importance. Among the most ubiquitous examples are touchscreens that most people are familiar with from their smartphones. The quality of such an HMI can be improved by adding haptic feedback-an imitation of using mechanical buttons-to the touchscreen. Thin-film actuators on the basis of electro-mechanically active polymers (EAPs), with the electroactive material sandwiched between two compliant electrodes, offer a promising technology for haptic surfaces. In thin-film technology, the thickness and the number of stacked layers of the electroactive dielectric are key parameters for tuning a system. Therefore, we have experimentally investigated the influence of the thickness of a single EAP layer on the electrical and the electro-mechanical performance of the transducer. In order to achieve high electro-mechanical actuator outputs, we have employed relaxor-ferroelectric ter-fluoropolymers that can be screen-printed. By means of a model-based approach, we have also directly compared single- and multi-layer actuators, thus providing guidelines for optimized transducer configurations with respect to the system requirements of haptic applications for which the operation frequency is of particular importance.
The effects of thermal processing on the micro- and nanostructural features and thus also on the relaxor-ferroelectric properties of a P(VDF-TrFE-CFE) terpolymer were investigated in detail by means of dielectric experiments, such as dielectric relaxation spectroscopy (DRS), dielectric hysteresis loops, and thermally stimulated depolarization currents (TSDCs). The results were correlated with those obtained from differential scanning calorimetry (DSC), wide-angle X-ray diffraction (WAXD), and Fourier-transform infrared spectroscopy (FTIR). The results from DRS and DSC show that annealing reduces the Curie transition temperature of the terpolymer, whereas the results from WAXD scans and FTIR spectra help to understand the shift in the Curie transition temperatures as a result of reducing the ferroelectric phase fraction, which by default exists even in terpolymers with relatively high CFE contents. In addition, the TSDC traces reveal that annealing has a similar effect on the midtemperature transition by altering the fraction of constrained amorphous phase at the interphase between the crystalline and the amorphous regions. Changes in the transition temperatures are in turn related to the behavior of the hysteresis curves on differently heat-treated samples. During heating, evolution of the hysteresis curves from ferroelectric to relaxor-ferroelectric, first exhibiting single hysteresis loops and then double hysteresis loops near the Curie transition of the sample, is observed. When comparing the dielectric-hysteresis loops obtained at various temperatures, we find that annealed terpolymer films show higher electric-displacement values and lower coercive fields than the nonannealed sample, irrespective of the measurement temperature, and also exhibit ideal relaxor- ferroelectric behavior at ambient temperatures, which makes them excellent candidates for applications at or near room temperature. By tailoring the annealing conditions, it has been shown that the application temperature could be increased by fine tuning the induced micro- and nanostructures.
Tailoring the secondary surface morphology of electro-spun nanofibers has been highly desired, as such delicate structures equip nanofibers with distinct functions. Here, we report a simple strategy to directly reconstruct the surface of polyvinyl alcohol/polyvinylpyrrolidone (PVA/PVP) nanofibers by water evaporation. The roughness and diameter of the nanofibers depend on the temperature during vacuum drying. Surface changes of the nanofibers from smooth to rough were observed at 55 degrees C, with a significant drop in nanofiber diameter. We attribute the formation of the secondary surface morphology to the intermolecular forces in the water vapor, including capillary and the compression forces, on the basis of the results from the Fourier-transform infrared (FTIR) and X-ray photoelectron (XPS) spectroscopy. The strategy is universally effective for various electro-spun polymer nanofibers, thus opening up avenues toward more detailed and sophisticated structure design and implementation for nanofibers.
Poly(vinylidenefluoride-trifluoroethylene)-based (P(VDF-TrFE)-based) terpolymers represent a new class of electroactive polymer materials that are relaxor-ferroelectric (RF) polymers and that offer unique and attractive property combinations in comparison with conventional ferroelectric polymers. The RF state is achieved by introducing a fluorine-containing termonomer as a "defect" into the ferroelectric P(VDF-TrFE) copolymer, which reduces the interaction between the VDF/TrFE dipoles. The resulting terpolymer exhibits a low Curie transition temperature and small remanent and coercive fields yielding a slim hysteresis loop that is typical for RF materials. Though the macroscopic behavior is similar to RF ceramics, the mechanisms of relaxor ferroelectricity in semi-crystalline polymers are different and not fully understood yet. Structure-property relationships play an important role in RF terpolymers, as they govern the final RF properties. Hence, a review of important characteristics, previous studies and relevant developments of P(VDF-TrFE)-based terfluoropolymers with either chlorofluoroethylene (CFE) or chlorotrifluoroethylene (CTFE) as the termonomer is deemed useful. The role of the termonomer and of its composition, as well as the effects of the processing conditions on the semi-crystalline structure which in turn affects the final RF properties are discussed in detail. In addition, the presence of noteworthy transition(s) in the mid-temperature range and the influence of preparation conditions on those transitions are reviewed. A better understanding of the fundamental aspects affecting the semi-crystalline structures will help to elucidate the nature of RF activity in VDF-based terpolymers and also help to further improve their applications-relevant electroactive properties.
Three poly(tetrafluoroethylene-hexafluoropropylene-vinylidenefluoride) (TFE-HFP-VDF or THV) terpolymers (Dyneon (R)) with different monomer ratios are investigated to demonstrate the concept of "modified" PTFE for space-charge electrets. HFP and VDF monomers distort the highly ordered PTFE molecules, which effectively enhances processability and adversely affects space-charge storage. Particularly, VDF component renders the material polar and probably also more conductive, partially undermining the space-charge-storage capabilities of PTFE. Nevertheless, the terpolymer THV815 with a TFE/HFP/VDF wt% ratio of 76.1/10.9/13 combines easy processability and relatively good space-charge stability. Our results shed light on novel concepts for space-charge electret materials with enhanced processing properties and reasonable charge-storage capabilities.
Here, a promising approach for producing piezo-polymer transducers in a one-step process is presented. Using 3D-printing technology and polypropylene (PP) filaments, we are able to print a two-layered film structure with regular cavities of precisely controlled size and shape. It is found that the 3D-printed samples exhibit piezoelectric coefficients up to 200 pC/N, similar to those of other PP ferroelectrets, and their temporal and thermal behavior is in good agreement with those known of PP ferroelectrets. The piezoelectric response strongly decreases for applied pressures above 20 kPa, as the pressure in the air-filled cavities strongly influences the overall elastic modulus of ferroelectrets.
A double-layer transcrystalline polypropylene (PP) film with a flat central interface layer between its two transcrystalline layers is obtained by recrystallization from the melt between two polytetrafluoroethylene (PTFE) surfaces on both sides of the PP film. Its electret properties are studied and compared with those of a single-layer transcrystalline PP film re-crystallized in contact with only one PTFE surface. Within experimental uncertainty, the two types of transcrystalline films exhibit the same thermal properties and crystallinities. After thermal poling, however, two hetero-charge layers of opposite polarity are found on the internal interfaces of the double-layer transcrystalline films and may together be considered as micrometer-sized dipoles. The unexpected phenomenon does not occur in single-layer transcrystalline samples without a central interface layer, suggesting that the interfaces between the transcrystalline layers and the micrometer-thick central interface layer may be the origin of deeper traps rather than the crystalline structures in the transcrystallites or the spherulites. The origin of the interfacial charges was also studied by means of an injection-blocking charging method, which revealed that intrinsic charge carriers introduced during recrystallization are most likely responsible for the interfacial charges. It is fascinating that a material as familiar as PP can exhibit such intriguing properties with a special bipolar space-charge polarization across the central interface layer after quasi-epitaxial surface moulding into a double-layer transcrystalline form. In addition to applications in electret (micro-)devices for electro-mechanical transduction, the highly ordered structures may also be employed as a new paradigm for studying charge storage and transport in polymer electrets and in dielectrics for DC electrical insulation.
Spherulite-related space-charge electret properties of polypropylene (PP) have been widely discussed in the past decades. In the present paper, a less-common crystalline structure in PP-transcrystalline PP-is studied regarding its electret behavior in comparison with the typical spherulitic morphology. Polarized light microscopy and differential scanning calorimetry were employed to characterize the crystallite types and crystallinities of transcrystalline and spherulitic PP. Their electret functionality is investigated by means of thermally stimulated discharge experiments, where the cross-over phenomenon is observed on transcrystalline PP films, whereas surface-potential saturation and undercharging on the surface occur on the spherulitic samples. Besides, an asymmetrical behavior of positive and negative surface-charge stabilities is found on PP with spherulites, the negatively charged spherulitic surfaces show a better charge stability. It is shown that PP electrets are very sensitive to changes in the microscopic crystalline structures and their interfaces as well as in the molecular conformations controlled through adjustments of the respective processing steps. In addition, surface and bulk nanocomposites of PP or low-density polyethylene with inorganic particles are included in the comparison. In view of recent developments in the areas of PP-based electret-fiber filters and cellular-foam ferroelectrets, the observed changes in the charge-storage properties may have particular relevance, as the required film, fiber, or foam processing might significantly modify crystalline morphologies and nano-scale interfaces in PP electrets. Limitations in the charge-storage capabilities of interface structures may also be of interest in the context of high-voltage electrical-insulation materials where reduced space-charge accumulation and slightly increased charge transport can be advantageous.
A new variant of the Laser-Induced Pressure-Pulse (LIPP) method for repeatable, time-resolved space-charge profile measurements is proposed and demonstrated. Automated deposition of a fresh laser-target film before each illumination leads to good repeatability of the LIPP and thus allows for the detection of time-resolved changes in the space-charge distribution over many hours. We describe and discuss the experimental setup and its features, compare the repeatability of the LIPP measurements on the same sample without and with re-preparation of the test cell, and present the time-resolved evolution of the space-charge profile in a two-layer arrangement of a silicone-grease and a silicone-elastomer film as an example. Finally, the temperature dependence of the space-charge evolution during polarization under high voltage and during depolarization in short circuit is shown. Possible uses and future developments of the new LIPP approach are also discussed.
Here, piezoelectric transducers consisting of a P(VDF-TrFE) layer with either silver or PEDOT:PSS screen-printed electrodes are studied. The influence of electrodes on the dielectric and electroacoustic properties are studied in dielectric-spectroscopy and ferroelectric-hysteresis measurements. Only when both the bottom and the top electrodes are made of silver, the typical dielectric relaxation of the P(VDF-TrFE) layer is clearly observed. When one or two of the electrodes are of PEDOT:PSS, a Debye-like relaxation is present. Compared with silver electrodes, PEDOT:PSS electrodes allow for moderate self-healing. Consequently, samples with bottom and top PEDOT:PSS electrodes can be poled to saturation, while samples with silver electrodes can hardly be poled to saturation due to destructive electric breakdown. Acoustic transducer measurements show that silver electrodes facilitate higher and broader frequency operation, while PEDOT:PSS electrodes bring slightly lower total harmonic distortion. Overall, the acoustic performance shows no significant deviations between differently electroded samples so that silver electrodes do not offer any advantages for the transducers studied here due to their much higher tendency for destructive electric breakdown.
The prehistory of electrets is not known yet, but it is quite likely that the electrostatic charging behavior of amber (Greek: τò ηλεκτρoν, i.e., “electron”) already was familiar to people in ancient cultures (China, Egypt, Greece, etc.), before the Greek philosopher and scientist Thales of Miletus (6th century BCE)-or rather his disciples and followers-reported it in writing (cf. Figure 1). More than two millennia later, William Gilbert (1544–1603), the physician of Queen Elizabeth I, coined the term “electric” in his book De Magnete, Magneticisque Corporibus, et de Magno Magnete Tellure (1600) for dielectric materials that attract like amber and that included sulfur and glass [1]. The second half of the 18th century saw the invention of the electrophorus or electrophore [2], a capacitive electret device, in 1762 by Johan Carl Wilcke (1732–1796).
Bipolar electrets from polypropylene (PP) are essential, e.g., in electret air filters and in cellular-foam ferroelectrets. Therefore, the mechanism of surface-charge stability enhancement on PP electrets via orthophosphoric-acid surface treatment is investigated in detail. It is shown that the significant charge-stability enhancement can be mainly attributed to deeper surface traps originating from deposited chemicals and topographic features on the modified surfaces. Thermally stimulated discharge of chemically treated and non-treated PP films with different surface-charge densities is used to test the limits of the newly formed deep traps in terms of the capacity for hosting surface charges. When the initial surface-charge density is very high, more charges are forced into shallower original traps on the surface or in the bulk of the treated PP samples, reducing the effect of the deeper surface traps brought by the surface modification. The well-known crossover phenomenon (of the surface-charge decay curves) has been observed between modified PP electrets charged to +/- 2kV and to +/- 3kV. Acoustically probed charge distributions in the thickness direction of PP electrets at different stages of thermal discharging indicate that the deep surface trapping sites may have preference for negative charges, resulting in the observed asymmetric charge stability of the modified PP films.
Polyvinylidene fluoride (PVDF)-based copolymers with tetrafluoroethylene (P(VDF-TFE)), trifluoroethylene (P(VDF-TrFE)) or hexafluoropropylene (P(VDF-HFP)) are of strong interest due to the underlying fundamental mechanisms and the potential ferro-, pyro- and piezo-electrical applications. Their flexibility and their adaptability to various shapes are advantageous in comparison to inorganic ferroelectrics. Here, we study the influence of stretching temperature on the crystalline phases and the dielectric properties in P(VDF-TFE) films by means of Dielectric Relaxation Spectroscopy (DRS), Fourier-Transform InfraRed spectroscopy (FTIR), Wide-Angle X-ray Diffraction (WAXD), Differential Scanning Calorimetry (DSC) and Dynamic Mechanical Analysis (DMA). Especially, the effect of stretching and the influence of the temperature of stretching on the mid-temperature (T-mid) transition are studied in detail. The results show that stretching has a similar effect as that on PVDF, and we observe an increase in the fraction of ferroelectric beta-phase with a simultaneous increment in both melting point (T-m) and crystallinity (chi(c)) of the copolymer. While an increase in the stretching temperature does not have a profound impact on the amount of ferroelectric phase, the stability of the ferroelectric phase seems to improve - as seen in the reduction of the Full Width at Half Maximum (FWHM) of the WAXD peaks in both parallel and perpendicular directions to the molecular chain axis. The observation is also supported by the reduction of dissipation losses with an increase in stretching temperature - as seen in DRS measurements. Finally, both stretching itself and the temperature of stretching affect the various molecular processes taking place in the temperature range of the T-mid transition.
Structural health monitoring activities are of primal importance for managing transport infrastructure, however most SHM methodologies are based on point-based sensors that have limitations in terms of their spatial positioning requirements, cost of development and measurement range. This paper describes the progress on the SENSKIN EC project whose objective is to develop a dielectric-elastomer and micro-electronics-based sensor, formed from a large highly extensible capacitance sensing membrane supported by advanced microelectronic circuitry, for monitoring transport infrastructure bridges. Such a sensor could provide spatial measurements of strain in excess of 10%. The actual sensor along with the data acquisition module, the communication module and power electronics are all integrated into a compact unit, the SENSKIN device, which is energy-efficient, requires simple signal processing and it is easy to install over various surface types. In terms of communication, SENSKIN devices interact with each other to form the SENSKIN system; a fully distributed and autonomous wireless sensor network that is able to self-monitor. SENSKIN system utilizes Delay-/Disruption-Tolerant Networking technologies to ensure that the strain measurements will be received by the base station even under extreme conditions where normal communications are disrupted. This paper describes the architecture of the SENSKIN system and the development and testing of the first SENSKIN prototype sensor, the data acquisition system, and the communication system.
During muscle contractions, radial-force distributions are generated on muscle surfaces due to muscle-volume changes, from which the corresponding body motions can be recorded by means of so-called force myography (FMG). Piezo- or ferroelectrets are flexible piezoelectric materials with attractive materials and sensing properties. In addition to several other applications, they are suitable for detecting force variations by means of wearable devices. In this paper, we prepared piezoelectrets from cellular polypropylene films by optimizing the fabrication procedures, and developed an FMG-recording system based on piezoelectret sensors. Different hand and wrist movements were successfully detected on able-bodied subjects with the FMG system. The FMG patterns were evaluated and identified by means of linear discriminant analysis and artificial neural network algorithms, and average motion-classification accuracies of 96.1% and 94.8%, respectively, were obtained. This paper demonstrates the feasibility of using piezoelectret-film sensors for FMG and may thus lead to alternative methods for detecting body motion and to related applications, e.g., in biomedical engineering or structural-health monitoring.