In this study, novel biodegradable long-segment fluorine-containing polyurethane (PU) was synthesized using 4,4′-diphenylmethane diisocyanate (MDI) and 1H,1H,10H,10H-perfluor-1,10-decanediol (PFD) as hard segment, and polycaprolactone diol (PCL) as a biodegradable soft segment. Nuclear magnetic resonance (NMR) was used to perform 1H NMR, 19F NMR, 19F–19F COSY, 1H–19F COSY, and HMBC analyses on the PFD/PU structures. The results, together with those from Fourier transform infrared spectroscopy (FTIR), verified that the PFD/PUs had been successfully synthesized. Additionally, the soft segment and PFD were changed, after which FTIR and XPS peak-differentiation-imitating analyses were employed to examine the relationship of the hydrogen bonding reaction between the PFD chain extender and PU. Subsequently, atomic force microscopy was used to investigate the changes in the microphase structure between the PFD chain extender and PU, after which the effects of the thermal properties between them were investigated through thermogravimetric analysis, differential scanning calorimetry, and dynamic mechanical analysis. Finally, the effects of the PFD chain extender on the mechanical properties of the PU were investigated through a tensile strength test.
In this paper, a side-by-side, dual-nozzle electrospinning process was used to prepare a flexible hybrid electronics (FHE) material with excellent stretchable properties. A highly stable electrical conductivity was also imparted to the resulting membrane electrodes using silver nanoparticles (AgNPs) and carbon-based nanomaterials of different structures. The AgNP/carbon-based nanomaterials were coated onto bicomponent polymer nanofibers (composed of polyurethane (PU) and polyvinylidene difluoride (PVDF)) on the nanofiber membrane. The FHE nanofiber electrodes were finally integrated into clothing designed to accurately measure human body sensing signals (e.g., electrocardiography (ECG) and electromyography (EMG) signals). To effectively increase the high electrical conductivity, a polymer-type dispersant (polyisobutylene-b-poly(oxyethylene)-b-polyisobutylene, a triblock copolymer) was used to effectively and stably disperse AgNPs with different particle sizes and carbon-based nanomaterials with different geometric dimensions (e.g., zero-dimensional carbon black, one-dimensional carbon nanotubes, and two-dimensional graphene) through non-covalent adsorption. Moreover, the bicomponent PVDF–PU nanofibers were immersed in a mixed dispersant of AgNPs and carbon-based nanomaterials at low concentrations, and thermal post-treatment was conducted to improve the electrical conductivity. The AgNP/graphene oxide (GO) nanofiber electrode exhibited a continuous phase with a stable material microstructure after 5000 repetitions of 50% tension–tension fatigue testing. The waveform pattern obtained from the proposed AgNP/GO nanofiber electrode was compared with those of traditional ECG and EMG electrodes. The nanofiber web electrode treated with organic/inorganic mixed dispersants and verified via tests of its electrical and fatigue properties was found to be suitable for long-term ECG and EMG monitoring, and it has excellent potential in wearable smart sensors.
This research has successfully synthesized highly flexible and conductive nanohybrid electrode films. Nanodispersion and stabilization of silver nanoparticles (AgNPs) were achieved via non-covalent adsorption and with an organic polymeric dispersant and inorganic carbon-based nanomaterials—nano-carbon black (CB), carbon nanotubes (CNT), and graphene oxide (GO). The new polymeric dispersant—polyisobutylene-b-poly(oxyethylene)-b-polyisobutylene (PIB-POE-PIB) triblock copolymer—could stabilize AgNPs. Simultaneously, this stabilization was conducted through the addition of mixed organic/inorganic dispersants based on zero- (0D), one- (1D), and two-dimensional (2D) nanomaterials, namely CB, CNT, and GO. Furthermore, the dispersion solution was evenly coated/mixed onto polymeric substrates, and the products were heated. As a result, highly conductive thin-film materials (with a surface electrical resistance of approximately 10−2 Ω/sq) were eventually acquired. The results indicated that 2D carbon-based nanomaterials (GO) could stabilize AgNPs more effectively during their reductNion and, hence, generate particles with the smallest sizes, as the COO− functional groups of GO are evenly distributed. The optimal AgNPs/PIB-POE-PIB/GO ratio was 20:20:1. Furthermore, the flexible electrode layers were successfully manufactured and applied in wearable electronic sensors to generate electrocardiograms (ECGs). ECGs were, thereafter, successfully obtained.
A flexible hybrid substrate was developed by affixing gold nanoparticles (AuNPs) onto the surface of two-dimensional nanomica platelets (NMPs). The substrate was successfully used in biosensors with high efficiency and high selectivity through surface-enhanced Raman scattering (SERS). By controlling the amphiphilicity of the hybrid substrate, the flexible substrate was made highly selective toward biomolecules. Four different SERS substrate systems were constructed, including intercalated mica, exfoliated NMPs, hydrophilic exfoliated NMPs, and hydrophobic exfoliated NMPs. NMPs were only 1 nm thick. AuNPs adsorbed on both sides of NMPs and thus created excellent threedimensional hot junction effects in the z-axis direction. For the detection of adenine in DNA, a satisfactory Raman enhancement factor (EF) of up to 8.9 × 10 6 was achieved with the detection limit as low as 10 −8 M. Subsequently, the AuNP/NMP hybrids were adopted to rapidly detect hydrophilic Staphylococcus hominis and hydrophobic Escherichia coli. The AuNP/PIB−POE−PIB/NMP nanohybrid was concurrently hydrophilic and hydrophobic. This amphiphilic property greatly enhanced the detection selectivity and signal intensity for hydrophilic or hydrophobic bacteria. Overall, AuNPs/PIB−POE−PIB/NMPs developed as SERS substrates enable rapid, sensitive biodetection.
This study created water polyurethane (WPU) prepolymer by using isophorone diisocyanate, castor oil, dimethylolpropionic acid, and triethanolamine (TEA) as the hard segment, soft segment, hydrophilic group, and neutralizer, respectively. TEA, deionized water, and carbon black (CB) were added to the prepolymer under high-speed rotation to create an environmentally friendly vegetable-oil-based polyurethane. CB served as the fortifier and promoter of microphase separation. Fourier transform infrared spectroscopy was performed to elucidate the role of H-bond interactions within the CB/WPUs. Additionally, atomic force microscopy was conducted to determine the influence of H-bond interactions on the degree of microphase separation in the WPU. Furthermore, this study used four-point probe observation to discover the materials’ conductivity of CB in the WPU. Thermogravimetric analysis and dynamic mechanical analysis were performed to measure the thermal properties of the CB/WPUs. The mechanical properties of CB/WPUs were measured using a tensile testing machine. The CB/WPUs were also soaked in 1 wt.% NaOH solution for different amounts of time to determine the degradation properties of the CB/WPUs. Finally, scanning electron microscopy was performed to observe the topography of the CB/WPUs after degradation.
In this study, lead zirconate titanate (PZT) ceramic particles were added for further improvement. PZT belongs to the perovskite family and exhibits good piezoelectricity. Thus, it was added in this experiment to enhance the piezoelectric response of the poly(vinylidenefluoride- co -trifluoroethylene) (PVDF-TrFE) copolymer, which produced a voltage output of 1.958 V under a cyclic pressure of 290 N. In addition, to further disperse the PZT particles in the PVDF-TrFE matrix, tetradecylphosphonic acid (TDPA) was synthesized and employed to modify the PZT surface, after which the surface-modified PZT (m-PZT) particles were added to the PVDF-TrFE matrix. The TDPA on the PZT surface made it difficult for the particles to aggregate, allowing them to disperse in the polymer solution more stably. In this way, the PZT particles with piezoelectric responses could be uniformly dispersed in the PVDF-TrFE film, thereby further enhancing its overall piezoelectric response. The test results showed that upon the addition of 10 wt % m-PZT, the piezoelectric coefficient of m-PZT/PVDF-TrFE 10 wt % was 27 pC/N; and under a cyclic pressure of 290 N, the output voltage reached 3.426 V, which demonstrated a better piezoelectric response than the polymer film with the original PZT particles. Furthermore, the piezoelectric coefficient of m-PZT/PVDF-TrFE 10 wt % was 27.1 pC/N. This was exhibited by maintaining a piezoelectric coefficient of 26.8 pC/N after 2000 cycles. Overall, a flexible piezoelectric film with a high piezoelectric coefficient was prepared by following a simple fabrication process, which showed that this film possesses great commercial potential.
In this study, heat and polarization treatments were applied to poly(vinylidenefluoride-co-trifluoroethylene (PVDF-TrFE) films to improve their crystallinity and piezoelectric effect. Carbon-based nanomaterials (CBNs) of multiple dimensions (i.e., modified zero-dimensional (0D) carbon black (OCB), one-dimensional (1D) modified carbon nanotubes (CNT–COOH) and two-dimensional (2D) graphene oxide (GO)) were added to the copolymer to study the effects of different CBN dimensions on the crystallinity and piezoelectric effect of PVDF-TrFE films. Additionally, amphiphilic polymeric dispersants were added to improve the dispersibility of CBNs; the dispersant was synthesized by the amidation, and imidization reactions of styrene-maleic anhydride copolymer (SMAz) and polyoxyalkylene amine (M1000). Polymer solutions with different ratios of CBN to dispersant (z = 10:1, 5:1, 1:1, 1:5, 1:10) were prepared. The enhanced dispersibility enabled the fluorine atoms in the PVDF-TrFE molecular chain to more efficiently form hydrogen bonds with the –COOH group in the CBN, thereby increasing the content of the β crystal phase (the origin of the piezoelectric effect) of the film. Therefore, the resulting film exhibited a higher output voltage on the application side and better sensitivity on the sensing element. The addition of CNT–COOH and polymeric dispersants increased the β-phase content in PVDF-TrFE from 73.6% to 86.4%, which in turn raised the piezoelectric coefficient from 19.8 ± 1.0 to 26.4 ± 1.3 pC/N. The composite film-based pressure sensor also exhibited a high degree of sensitivity, which is expected to have commercial potential in the future.
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