Excellent Piezoelectric Performance Research Articles

Novel 3D printed PZT-based piezoceramics for piezoelectric energy harvesting via digital light processing

Structure optimization is a highly effective way for enhancing the power output of piezoceramics. However, due to the high hardness and brittleness of these materials, traditional manufacturing methods are limited in their ability to optimize structures. Moreover, achieving new designs using the emerging digital light processing (DLP) technology is hindered by poor curing performance of piezoceramic slurry. To overcome these issues, this study proposes an innovative strategy of using the original powders as printing materials for DLP technology. Notably, the use of lead carbonate powders, rather than lead oxide, significantly improves the curing characteristics and printability of ceramic slurry. Additionally, lanthanum oxide powders are introduced as dopants to enhance the electrical properties of PZT ceramics. The printed piezoceramics exhibit excellent piezoelectric and dielectric performance under optimal La3+ content, coupled with superior transduction coefficient, electromechanical coupling factor and output voltages and currents. Our findings suggest a groundbreaking approach for fabricating piezoceramics with high energy-harvesting performance and complicated designed structure via digital light processing.

Tuning the Piezoelectric Performance of K0.5Na0.5NbO3 through Li Doping: Insights from Structural, Elastic and Electronic Analyses.

The structural, elastic, piezoelectric, and electronic properties of Li-doped K0.5Na0.5NbO3 (K0.5-xNa0.5-yLix+yNbO3, KNN-L) are calculated. The properties of KNN-L are related to the Li-doping content and the replaced K or Na atoms. The bulk modulus, the shear modulus, and Young's modulus of KNN-L are mostly higher than those of KNN, and the hardness value increases. The Poisson ratio of KNN-L is lower than that of most KNN, and the ductility is reduced. All doped structures are direct band gap semiconductors. K0.5Na0.375Li0.125NbO3 has the largest piezoelectric charge constant, d33 = 44.72 pC/N, in the respective structures, which is 1.5 fold that of K0.5Na0.5NbO3 (29.15 pC/N). The excellent piezoelectric performance of Li-doping KNN-L was analyzed from the insights of elastic and electronic properties.

Thermal cycle stability and microstructure of Pb(Mg1/3Nb2/3)O3-PbTiO3 single crystals

The Pb(Mg1/3Nb2/3)O3-PbTiO3 (PMN-PT) ferroelectric single crystals have been commercially available as important components in medical ultrasound transducers due to their excellent piezoelectric and electromechanical coupling performance. The variation in piezoelectric and dielectric properties of PMN-PT single crystals with ambient temperature is an important application indicator. In this work, the PMN-PT single crystals after direct current poling (DCP) and alternating current poling (ACP) were subjected to the cyclic thermal treatment process. The thermal cycling stability and microstructural changes in PMN-PT single crystals were investigated. The ACP single crystals exhibit a higher dielectric constant ε33T/ε0 (6500–7600) and piezoelectric coefficient d33 (2100–2500 pC N−1) compared to the DCP single crystals (ε33T/ε0 of 4100–5000, d33 of 1200–1300 pC N−1). Under thermal cycling at 60 °C, the DCP and ACP single crystals exhibit good thermal cycling stability after 150 cycles. Microstructural observations show that the domain structure of the DCP single crystals exhibits “staggered domain walls, inhomogeneous domain size, variety of domain structure,” while the relatively homogeneous stripe-like domains were observed in the ACP single crystals. After thermal cycling, new fine striped domains appear in both the DCP and ACP single crystals due to the instability of rotated polarization, but the piezoelectric and dielectric properties are not greatly affected. This work provides an intensive understanding of the effects of thermal cycling on the domain structure, which is useful for applications.

Using multi-criteria decision-making approach for material alternatives in TiO2/P(VDF-TrFE)/PDMS based hybrid nanogenerator as a wearable device

P(VDF-TrFE)/TiO2/PDMS-based hybrid nanogenerators with excellent piezoelectric performance are of particular interest for the development of sensors, wearable devices, and low-cost biomechanical energy harvesters. In this work, hybrid nanogenerator (HNG) is designed to enhance the energy output by integrating piezoelectric and triboelectric effects. P(VDF-TrFE)/TiO2 nanocomposites are synthesized using electrospinning to design hybrid nanogenerator for energy harvesting from a manual activity. The hybrid nanogenerator device generated 5.36µA current across 10 MΩ resistor and 52V electric voltage. An analysis of the effect of varying TiO2 on hybrid nanogenerators is reported here for the first time. The best material for biomechanical energy harvesting applications is selected using a multi-criteria decision-making (MCDM) based material selection and optimization technique TODIM, along with a sensitivity study. SA-4 type nanocomposite is the most suitable material as per the TODIM approach. This nanogenerator shows better performance than most nanogenerators designed with complex and sophisticated approaches.

Attempt for excellent piezoelectric performance in Sb-free (K,Na)NbO3-based ceramics

Piezoelectric temperature stability is often a very important item for piezoelectric materials when putting them into practical applications like filters and ultrasonic transducers. Phase transitions of (K,Na)NbO3-based compositions that contain neither toxic Pb nor Sb elements were tailored to simultaneously acquire enhanced piezoelectric properties and good piezoelectric temperature stability in this study. Specifically, dense 0.94(K0·48Na0.52)NbO3-0.03BaZrO3-0.01BaSnO3-0.02(Bi0·5Na0.5)ZrO3 ceramic and its further compositionally modified one by 1 wt% MnO2 were prepared. Both of these two ceramics display quite weak piezoelectric temperature dependence in the usage temperature range between −30 °C–100 °C, but the one modified by MnO2 has the significantly improved piezoelectric properties with a high piezoelectric coefficient d33 of 310 pC/N and large electromechanical coupling factors kp and k33 of 0.57 and 0.73 at room temperature. The obtained excellent piezoelectric performance is considered to be associated closely with the stable piezoelectric characteristic of the orthorhombic phase and the diffused rhombohedral-orthorhombic and orthorhombic-tetragonal phase transitions.

Excellent temperature stability of piezoelectric properties in PbNb2O6‐based ceramics up to 450°C

AbstractDense (Pb0.92Ba0.08)Nb2O6‐xmol% MnO2 with 0.25 wt% TiO2 ceramics with a single orthorhombic phase were synthesized through a conventional solid‐state reaction method. Excellent piezoelectric performance (d33 = 90 pC/N) and low dielectric loss (tan δ = 0.5%) are achieved in Mn‐doped samples. Interestingly, the dielectric anomalies are observed in the temperature range of 300–400°C, which could be completely suppressed through Mn doping. The dielectric anomalies are associated with thermally activated domain wall motion, which could be constrained by the defect dipoles produced by Mn doping. More importantly, all samples experience about 12% performance degradation below 300°C, attributed to an accelerated aging process at elevated temperatures. After thermal aging, the samples exhibit excellent performance stability within the temperature range of 25–450°C, showing no further degradation. The results indicate that the PbNb2O6‐based ceramics are promising high‐temperature piezoelectric materials for piezoelectric devices operating at temperatures up to 450°C.

Enhanced energy harvesting performance of piezoelectric cantilever using (Bi,Sm)ScO3-PbTiO3 ceramics textured by microstructural engineering

Energy harvesting performance of piezoelectric cantilevers using untextured and textured piezoelectric 0.38(Bi0.97Sm0.03)ScO3-0.62PbTiO3 (0.38BSS-0.62PT) ceramics was evaluated and subsequently, results were compared to demonstrate effect of microstructurally engineered texture. The textured 0.38BSS-0.62PT ceramic showed figures of merit and conversion efficiency superior to those of the untextured case. Energy density (d31 × g31) was especially enhanced for the textured 0.38BSS-0.62PT ceramic, which can lead to excellent piezoelectric energy harvesting performance. The output power of the piezoelectric cantilever using textured 0.38BSS-0.62PT ceramic was 8.46 mW at load resistance of 70 kΩ, corresponding to a power density of 12.80 mW/cm3. This was sufficient to fully charge a 10 V capacitor in 280 s.

Preparation, spectroscopic, thermal properties, and laser performances of ordered Nd3+: Ca3TaGa2.1Al0.9Si2O14 crystal

Langasite crystals with an ordered structure of space group P321 are well known for their excellent piezoelectric and nonlinear optics performance. In this paper, a novel Nd3+: Ca3TaGa2.1Al0.9Si2O14 (Nd: CTGAS) crystal with an ordered structure of space group P321 was successfully grown using the Czochralski method, which could be used as self-laser photoelastic modulators. The thermal behaviour, polarized spectroscopy, and fluorescence lifetime were characterized in detail, and excellent spectroscopic and laser properties were presented. The full width at half of the maximum (FWHM) of the 0.8 μm absorption band was 23.5 nm for σ-polarized and 15.3 nm for π-polarized. The emission spectra had inhomogeneous broadening; the maximum emission cross-section was 7.50 × 10−20 cm2 at 1065 nm with FWHM of 14.3 nm and 2.35 × 10−20 cm2 at 1346 nm with FWHM of 28.3 nm. The fluorescence lifetime at 1065 nm was 280.8 μs. The diode-pumped continuous-wave (CW) laser operation at 1.06 μm was achieved in Nd: CTGAS crystal, an output power of 1.77 W was obtained at the absorbed pump power of 5.5 W, the slope efficiency was 35.0 %, and the optical conversion efficiency was 32.2 %. A 1.35 μm CW laser operation with a slope efficiency of 12.0 % was realized in z-cut Nd: CTGAS crystal.

Self-poled PVDF/recycled cellulose composite fibers utilizing cellulose nanocrystals to induce PVDF β-phase formation through wet-spinning as a flexible fabric piezoelectric sensor

In general, PVDF (Polyvinylidene fluoride) needs polarization treatment to exhibit its piezoelectric properties. Introducing nanofillers or applying stretching during the processing can promote the β-phase transformation in PVDF, achieving self-polarization. Herein, by incorporation of cellulose nanocrystals (CNCs), continuous β-phase enriched PVDF/cellulose composite fibers are prepared via wet spinning and drawing, in which the cellulose is recycled from waste cotton textiles to improve the wet spinnability of PVDF and reduce the cost. The obtained composite fibers are woven into fabrics and subsequently assembled into a flexible sensor, exhibiting excellent piezoelectric performance (d33 = 26.2 pC/N) without requiring additional polarization treatment. It generates an open-circuit voltage of 12 V and a short-circuit current of 100nA, much higher than those of the previously reported piezoelectric PVDF sensors with high-voltage polarization. This fabric-based flexible sensor also exhibits notable characteristics, including stable output signals and heightened sensitivity, thereby fulfilling the demands for monitoring both minute and extensive human movements. Furthermore, it shows great potential for widespread use in sound sensing for human-machine interfaces. The self-poled PVDF composite fibers offer the advantage of being easily woven together with other fiber materials, which contributes towards the development of self-powered flexible piezoelectric fabric sensors.

Design, analysis and testing of monometallic plate stepped broadband high sensitivity transducer

In order to improve the performance of the sonar system, a stepped broadband high-sensitivity hydroacoustic transducer is developed. Through theoretical analysis and finite element simulation, the feasibility of expanding the operating bandwidth and improving the sensitivity of the monometallic plate stepped piezoelectric material sensitive element is analyzed, and the dimensional parameters of this sensitive element are optimized. Compared with the traditional composite material, the sensitive element has excellent piezoelectric performance, with broadband and high sensitivity properties. The monometallic plate stepped piezoelectric material transducer and the same size stepped composite transducer were prepared, and their hydroacoustic performance was tested. The test results show that the monometallic plate stepped piezoelectric material transducer has far superior sensitivity performance than the same size stepped composite transducer and also has broadband performance. The peak transmits voltage response of the monometallic plate stepped transducer is 166 dB, and the −3 dB bandwidth reaches 60 kHz; the peak receives sensitivity is −183 dB, and the −3 dB bandwidth reaches 55 kHz, which can effectively improve the performance of the sonar system.

Enhanced piezoelectricity of Cu-doped K(Ta,Nb)O3 single crystals

As a class of solid solution material, K(Ta,Nb)O3 (KTN) single crystals have attracted significant interest due to their excellent piezoelectric and electro-optic performance. In this study, the piezoelectric properties of KTN were improved through Cu doping. Utilizing the advantages of composition-regulating phase transition, a large, high-quality Cu:KTN crystal measuring 30 mm × 25 mm × 20 mm in size was grown using the improved top seeded solution growth method. Cu-doped KTN exhibited better piezoelectric properties than pure KTN, and the full matrix parameters were investigated. Excellent dielectric, piezoelectric, and electromechanical coupling responses (ε11T∼ 2,136, d33∼303 pC/N, kt∼0.515, and k33∼0.672) were successfully obtained. To realize the optimized orientation of the piezoelectric properties, the orientation dependence of the single domain properties was investigated, and the mechanism of Cu doping to improve piezoelectric properties was explored. We found that 0.36% (in mass) Cu doped crystal consisted of A-site substitution, following ferroelectric and domain analysis. The small ferroelectric domain sizes led to a large domain wall mobility rate and high domain wall density, which contributed to high piezoelectric properties. This work revealed the effect of A-position doping on piezoelectric properties and provided a theoretical and experimental foundation for the performance optimization of KTN-based materials.

Micromachining of High-Quality PMN-PT/Epoxy 1-3 Composite for High-Frequency (>30 MHz) Ultrasonic Transducer Applications.

Fabricating PMN-PT composites, the core component of high-frequency (>30 MHz) transducers, remains challenging due to their poor machinability and ultra-small kerfs. This urgent problem is significantly impeding the development of PMN-PT ultrasonic transducers for use in clinical research, biomedical sciences, and nondestructive testing. In this study, high-quality PMN-0.3PT/epoxy 1-3 composites at 30 MHz and 50 MHz were manufactured using a modified picosecond (1.5 ps) laser technique. Their performance was thoroughly analyzed, which was comparable to that with low-stress dry plasma etching. There were fewer microcracks around PMN-PT pillars. The minimum kerf was less than 4.5 μm and the highest aspect ratio was larger than 7.5. The micro domain morphology and hysteresis loops of PMN-PT pillars further confirmed that composites still maintained excellent piezoelectric performance and suffered fewer damages during laser cutting. The characterization results exhibited a large electromechanical coupling (>0.77), a high dielectric constant (>1600), and a relatively low acoustic impedance (<17 Mrayls). The ultrasonic transducers with centre frequencies of 30 MHz and 50 MHz were designed and prototyped to validate the performance of composites. The transducers showed broad bandwidth (>80%), high two-way insertion loss (>-23 dB), and imaging resolution superior to 40 μm. Finally, the C-scan experiments of IC chips were also used to further illustrate the applicability of transducers. These encouraging results further demonstrated that ultrafast laser technology will bring more accessible and affordable methods for fabricating high-frequency PMN-PT composite transducers with excellent performance.

Superior temperature stability of electromechanical properties and resonant frequency in PYN-PZT piezoelectric ceramics

In this study, the Pb(Yb1/2Nb1/2)O3 (PYN) relaxor with high Curie temperature (TC ∼300 °C) was incorporated into PbZrO3-PbTiO3 (PZ-PT) ceramics to form 0.1PYN-(1-x)PZ-xPT ternary ceramics, and their phase compositions were systematically investigated, providing the more detailed phase diagrams, dielectric, piezoelectric, and ferroelectric properties. Excellent piezoelectric performance (d33 ∼ 450 pC/N, d33* ∼714 pm/V), with high coercive field (EC ∼17.5 kV/cm) and TC (∼398 °C) were simultaneously achieved in the 0.1PYN-0.41PZ-0.49PT composition near the morphotropic phase boundary (MPB). The value of d33 × EC, which exhibits higher than commercial PZT ceramics, indicates its suitability for high-field excitation devices. Additionally, the temperature stability of the resonant frequency (fr) is qualitatively studied by analyzing the main factors influencing fr from a theoretical perspective. Superior stability is achieved in the 0.1PYN-0.38PZ-0.52PT composition (TC ∼ 405 °C) with tetragonal phase, and the temperature coefficient of resonant frequency (Δfr /fr25 °C) remains within 0.5% up to 300 °C, far outperformance than previous reports.

Multifunctional PVDF film embedded with surfactant assisted-graphene with excellent piezo-capacitance, piezoelectric and triboelectric properties for various applications

Herein, we have developed multifunctional, flexible and self-poled PVDF nanocomposite films incorporated with anionic surfactant-assisted graphene nanoplatelets (S-GNP). The synergistic effect of rapid cooling process and S-GNP promoted electroactive phase content up to >97% (β + γ) of PVDF and assisted in tuning the crystallinity, tensile and dielectric properties of the PVDF/S-GNP nanocomposite (S-PGN-X) films. A flexible piezo-capacitance based pressure sensor offered an excellent response, quick recovery and high sensitivity (1.25 kPa−1) with a wide pressure sensing range (0.25–50 kPa). The sensor was integrated into a shoe sole to monitor the heel and toe pressure. Further, the S-PGN-X based triboelectric device showed excellent performance with a voltage output of >120 V and 175 μW/cm2 power density. The output of the device was sufficient to glow the LED lights, suggesting that it can be used as a sustainable power source for portable devices. Moreover, S-PGN-X based piezoelectric nanogenerator generated a voltage output of ∼19 V upon repeated application of pressure with a good power output of 1.35 μW/cm2. The piezoelectric nanogenerator could charge up a 3.3 μF capacitor up to 1.1 V under repeated finger impartation. Overall, the multifunctional S-PGN-X film with self-poling characteristics showed excellent piezo-capacitance, piezoelectric and triboelectric performance, which makes it a potential material for sensors, energy harvesting and portable electronic devices.

Coaxially oriented PVDF/MWCNT nanofibers as a high‐performance piezoelectric actuator

AbstractControlling the orientation of the carbon nanotubes inside a polymer matrix essentially improves their reinforcement effect even at small loading levels, which is attractive from the processing point of view. We inform the utilization of electrospinning to produce highly aligned small‐diameter polyvinylidene fluoride (PVDF) nanofibers where the multiwalled carbon nanotube (MWCNT) are coaxially aligned inside the PVDF nanofibers. The coaxially aligned MWCNTs arrange large numbers of contact sites with the polymer chains, thereby providing enhanced interfacial interactions, resulting in the superior effect of the MWCNTs on the crystalline structure and actuator response of the PVDF at low loading levels (0.06 wt.%). An effective α‐ to β‐phase conversion occurred through the synergistic effects of the electrospinning and MWCNTs, the β‐phase content reached 94%. Also, the degree of crystallinity increased up to 50% respecting the pure nanofibers. The bending actuation of the nanofibers was analyzed as the active layer of soft piezoelectric actuators in a unimorph configuration. The well‐aligned nanofibers showed better actuator deflection than the randomly oriented nanofibers. Comparing the PVDF nanofiber‐based actuators in the literature, our actuators exhibited excellent piezoelectric performance with high potential for practical applications.Highlights Highly aligned small‐diameter PVDF/CNT nanofibers produced by electrospinning. Axially aligned CNTs induce a great piezoelectric effect at low‐loading levels. The F(β) was 94%, and the crystallinity increased by 50% at only 0.06 wt% CNTs. Well‐aligned nanofibers showed better actuator response than the random ones. The soft actuators showed a higher performance than those in the literature.

Synergy of morphotropic phase boundary and internal bias fields to achieve high d33 and d33* simultaneously in lead-free BNT-based ceramics

It is difficult to obtain high d33 and d33* simultaneously in one piezoelectric ceramic system via a conventional method due to the conflicting structure–properties responding mechanism between the direct piezoelectric and converse piezoelectric effects. In this work, a synergistic approach of constructing morphotropic phase boundary and introducing the internal bias fields in (Bi0.5Na0.5)TiO3 ceramics is proposed through Sr2+ and Li+ doping for mitigating the conflict between d33 and d33*. By this strategy, both high d33 (197 pC/N) and d33* (1500 p.m./V) are realized in Srx(Bi1-xNa0.97-xLi0.03)0.5TiO3 when x = 0.24. The large d33 stems from rhombohedral and tetragonal (R3c and P4bm) phase coexistence. The internal bias field introduced by defect dipoles tends to counteract the effects of depolarization field, thus greatly aiding the external fields with higher actual excitation fields. The superposition of internal bias field, depolarization field and external fields yields strong asymmetry bipolar strain curves, thereby contributing to the large d33*. Thus, this work opens a new door for developing lead-free ceramics with excellent piezoelectric performance.

Simultaneously Achieving Large Piezoelectricity and Low Dielectric Loss in High-Temperature BiScO3-PbTiO3-Based Ceramics.

High-temperature piezoelectric materials are pivotal to technology applications fields including defense, aerospace, nuclear energy, and oil well logging. However, the acquisition of excellent piezoelectric properties is usually at the cost of temperature stability (reduced Curie temperature and increased high-temperature dielectric loss), which hinders the application of piezoelectric ceramics in harsh environments. In this study, we investigated the effect of Nb5+ donor and Mn2+/3+ acceptor doping on the dielectric and piezoelectric properties of BiScO3-PbTiO3 (BS-PT)-based ceramics. In contrast to the acceptor doping, it was found that the donor doping not only enhances the piezoelectric properties but also effectively suppresses the dielectric loss at a high temperature by reducing the oxygen vacancy concentration. Eventually, we simultaneously attained an excellent piezoelectric performance (d33 is 553 pC/N at room temperature and 1528 pC/N at 400 °C, respectively) and a low dielectric loss (less than 2% in the temperature range of 150-300 °C) but still with a high Curie temperature (TC ∼ 445 °C) in Nb5+-doped BS-PT ceramics. Furthermore, different in situ measurements were used to demonstrate the remarkable temperature stability up to a high depolarization temperature of ∼400 °C. This work represents significant progress in high-temperature piezoelectric materials and provides a guideline for future efforts on enhancing the piezoelectricity and suppressing the dielectric loss at high temperature.

Synthesis of novel flower-like Bi4Ti3O12/BiOCl heterojunctions with excellent piezoelectric photocatalytic performance

Photocatalysis technology can not only degrade pollutants by renewable solar energy, but also has enormous promise for resolving environmental issues. The piezoelectric field inside the piezoelectric material can be used as the driving force of charge separation to improve the photocatalytic activity. In order to study the catalytic effect of piezoelectric materials on photocatalysis, a flower-like Bi4Ti3O12/BiOCl (BTO/BOC) composite catalyst is prepared in this paper. The photogenerated carrier separation efficiency is characterized by electrochemical, PL and ESR tests. BOC's built-in electric field helps to facilitate the separation of photogenerated carrier, reducing the recombination rate and improving photocatalytic efficiency. The piezoelectric effect caused by ultrasonic vibration is coupled with the photocatalysis, which realizes the high efficiency co-catalysis of BTO/BOC piezoelectric photocatalyst. The polarized BTO/BOC heterojunction catalysts achieved a very high degradation efficiency (99.15 %) under piezo-photocatalysis. The degradation rates (k = 0.7494 min−1) are 1.74 and 8.19 times higher than photocatalysis (k = 0.4304 min−1) and piezoelectric catalysis (k = 0.0915 min−1), respectively. The investigation of the piezoelectric effect and photocatalysis's synergistic relationship is very significant.

Outstanding piezoelectric performance of BiScO3-PbTiO3-based ceramics over a wide high-temperature region

Piezoceramics with high piezoelectric performance in a wide elevated temperature range are the best potential stocks used in advanced high-temperature piezoelectric devices. Here, novel ternary perovskite piezoceramics of (0.997-x)BiScO3-xPbTiO3-0.003Bi(Zn2/3Nb1/3)O3 (BS-xPT-BZN) are synthesized and investigated. The morphotropic phase boundary (MPB) composition of the BS-xPT-BZN system is located at x = 0.625, which exhibits a high Curie temperature (TC) of 442 °C. More excitingly, the in-situ piezoelectric coefficient (d33) of the x = 0.625 MPB sample is not only as high as 558 pC/N at 200 °C, but also has a fluctuation rate of less than ± 10 % in the ultra-wide high-temperature range of 100 ∼ 308 °C. The above excellent comprehensive high-temperature piezoelectric performance should be attributed to the synergistic effect of composition-related MPB and dispersion characteristics and thermally stable ferroelectric domain state. The results demonstrate that BS-xPT-BZN ceramics can be used as very competitive perovskite piezoelectrics to construct piezoelectric devices for applications in harsh high-temperature environments.

Interface-engineered composite nanofibers for boosting piezoelectric outputs of polymeric nanogenerators

Polymeric piezoelectric nanogenerators (PENGs) hold great promise for flexible energy harvesters and self-powered sensors. However, achieving high piezoelectricity in inherently piezoelectric polymers while maintaining their flexibility remains a challenge. Herein, we propose a simple yet effective approach to fabricate flexible and cost-effective PENGs based on interface-engineered composite nanofibers of poly(vinylidene fluoride) (PVDF)/carbon nanotubes (CNTs) using electrospinning. Our strategy involves the incorporation of a tailor-made interfacial coupling agent, maleic anhydride grafted PVDF (PVDF-g-MA), onto PVDF/CNTs interfaces. This mild interface-engineering strategy not only promotes interfacial interactions within composites but also stabilizes electrospinning flow jets, yielding defect-free nanofibers. More importantly, the interfacial anchoring of PVDF-g-MA molecules promotes the preferential crystallization of electroactive β-phase within PVDF matrix. By incorporating a small quantity of PVDF-g-MA (up to 1.0 wt%), our approach significantly enhances piezoelectric outputs while preserving flexibility. This eliminates the need for excessive nanofiller usage that can sacrifice the flexibility associated with conventional methods. Remarkably, the resulting composite nanofiber-based PENGs exhibit excellent piezoelectric performance, generating high output voltages (10.6 V) and remarkable power density (3.15 µW/cm2) under tiny force stimuli. Our findings open new avenues for efficient and scalable fabrication of polymeric piezoelectric nanogenerators for flexible and wearable energy harvesting and self-powered sensing applications.