In recent years, flexible and sensitive pressure sensors are of extensive interest in healthcare monitoring, artificial intelligence, and national security. In this context, we report the synthetic procedure of a three-dimensional (3D) metal–organic framework (MOF) comprising cadmium (Cd) metals as nodes and isoniazid (INH) moieties as organic linkers (CdI2–INHCMe2) for designing self-polarized ferroelectret-based highly mechano-sensitive skin sensors. The as-synthesized MOF preferentially nucleates the stable piezoelectric β-phase in poly(vinylidene fluoride) (PVDF) and also gives rise to a porous ferroelectret composite film. Benefiting from the porous structure of 3D MOFs, composite ferroelectret film-based ultrasensitive pressure sensor (mechano-sensitivity of 8.52 V/kPa within 1 kPa pressure range) as well as high-throughput ( power density of 32 μW/cm2) mechanical energy harvester (MEH) has been designed. Simulation-based finite element method (FEM) analysis indicates that the geometrical stress confinement effect within the interpore region of the ferroelectret structure synergistically influences the mechano-electrical property of the MEH. In addition, 143 pC/N (∼4.5 times higher than commercial piezoelectric PVDF films) piezoelectric charge coefficient (d 33) magnitude and superior response time (t r ∼ 8 ms) of this composite ferroelectret film enable the detection of different physiological signals such as coughing, pronunciation, and gulping behavior, making it a promising candidate for early intervention of healthcare, which may play a significant role in accurate alert of influenza and chronic obstructive pulmonary disease (COPD)-related symptoms. In addition, MEH enables the tracking of the subtle pressure change in the wrist pulse, indicating its usefulness in effective mechano-sensitivity. Since the cardiovascular signal is one of the vital parameters that can determine the on-going physiological conditions, the wireless transmission of the detected wrist pulse signal has been demonstrated. All of these features coupled with wireless data transmission indicate the promising application of MOF-assisted composite ferroelectret films in noninvasive real-time remote healthcare monitoring.
The real-time application of piezoelectric nanogenerators (PNGs) under a harsh environment remains a challenge due to lower output performance and poor durability. Thus, the development of flexible, sensitive, and stable PNGs became a topic of interest to capture different human motions including gesture monitoring to speech recognition. Herein, a scalable approach is adapted where naphthylamine bridging a [Cd(II)-μ-I4] two-dimensional (2D) metal–organic framework (MOF)-reinforced poly(vinylidene fluoride) (PVDF) composite nanofibers mat is prepared to fabricate a flexible and sensitive composite piezoelectric nanogenerator (C-PNG). The needle-shaped MOF was successfully synthesized by the layering and diffusion of two different solutions. The incorporation of single-crystalline 2D MOF ensures a large content of electroactive phases (98%) with a resultant high-magnitude piezoelectric coefficient of 41 pC/N in a composite nanofibers mat due to the interfacial specific interaction with −CH2–/–CF2– dipoles of PVDF. As an outcome, C-PNG generates high electrical output (open-circuit voltage of 22 V and maximum power density of 24 μW/cm2) with a very fast response time (t r ≈ 5 ms) under periodic pressure imparting stimuli. Benefiting from bending and twisting functionality, C-PNG is capable of scavenging biomechanical energy by mimicking complex musculoskeletal motions that broaden its application in wearable electronics and fabric integrated medical devices. In addition, C-PNG also demonstrates an efficient acoustic vibration to electric energy conversion capability with an improved power density and acoustic sensitivity of 6.25 μW and 0.95 V/Pa, respectively. The overall energy conversion efficiency is sufficient to operate several consumer electronics without any energy storage unit. This acoustic observation is further validated by the finite element method-based theoretical simulation. Overall, the 2D MOF-based device design strategy opens up a new possibility to develop a human-motion compatible energy generator and a self-powered acoustic sensor to power up electronic gadgets as well as low-frequency noise detection.
Naphtheledicarboxylato ((NDC 2− ) bridged coordination polymers (CPs) along with (E)-1-methyl-2-(p-chlorophenylazo)imidazole (ClPai-Me) coordination to Co(II), [Co(∝-NDC) 0.5 (∝ 4 -NDC) 0.5 (ClPai-Me)]•0.5H 2 O (1), and to Zn(II), [Zn(∝-NDC) 0.5 (∝ 4 -NDC) 0.5 (ClPai-Me)]•0.5H 2 O (2), have been characterized. In the single crystal X-ray structure of 1, ClPai-Me chelates to the Co(II) ion by N(azo) and N(imidazolyl), whereas in compound 2, it acts as a monodentate N(imidazolyl) donor to the Zn(II) ion. The coordination atmosphere around Co(II) in the 1 ion is distorted octahedral CoN 2 O 4 , whereas in the case of 2, it is distorted square pyramidal ZnNO 4 . Compounds 1 and 2 exhibit the righthanded (P) and left-handed (M) one-dimensional helical chain. NDC −2 is serving as a bridge between two M(II) ions to constitute μ-NDC and four M(II) ions to construct μ 4 -NDC to assemble threedimensional polymers. Upon UV light (369 nm) irradiation, compound 2 shows trans-to-cis isomerization of -NN−C 6 H 4 −Clp both in the solid and solution state but 1 remains silent. Prolonged light irradiation in the solid state (film phase) does not change the coordinated ClPai-Me in complexes 1 and 2, whereas the free stage of ClPai-Me undergoes photoreduction of the −NN− bond and forms azo radicals with a concomitant permanent color change. The persistence of the radical has been characterized by electron paramagnetic resonance spectroscopy in the solid state at g = 2.009. The effective magnetic moment of 1 is 4.17 μ B at 300 K, Co(II) ion of S = 3/2.
A newly designed mixed-ligand coordination polymer [Zn4(bdc)4(ppmh)2(H2O)]n (1) (H2bdc = 1,4-benzene dicarboxylic acid, ppmh = N-pyridin-2-yl-N′-pyridin-4-ylmethylene-hydrazine) has been characterized using different physicochemical techniques. The structure has been confirmed by single crystal X-ray diffraction measurements. There are two pyridyl-N and one hydrazino-imine-N donor centers in ppmh, where two pyridyl-Ns bind simultaneously to two Zn(II) to serve as a bridging agent to form a coordination polymer. The 1,4-benzene dicarboxylato (bdc) is ligated via the aromatic dicarboxylato-O to form a one-dimensional (1D) chain. These two 1D chains about Zn(II) constitute a two-dimensional structure, which undergoes noncovalent interactions (C–H···π and π···π) to generate a three-dimensional supramolecular assembly. Electrical conductivity of 1 is higher by 1 order (1.37 × 10–6 S/cm) than that of the free ligand, ppmh (6.2 × 10–7 S/cm). Especially, the responsivity of the compound 1 was 56.21 mA/W, which is 11 times higher than that of the ligand ppmh (5.12 mA/W). The specific detectivity of the compound was 2.17 × 1010 Jones, which is also almost 10 times higher with respect to the specific detectivity of the ligand-based device (4.53 × 109 Jones). The results show that the compound can be valuable for optoelectronic fields. The biological studies suggest that compound 1 is antibacterial as well as a promising anticancer agent (LD50, 42.2 μg/mL against HepG2 cells), while ligands remain silent. Investigation of the mechanism of the cell killing activity of compound 1 accounts the generation of intracellular reactive oxygen species.
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