This review offers a critical overview of recent developments in lead-free piezoelectric materials and flexible device architectures for self-powered wearable and Internet of Things systems. It examines the scientific and technological rationale for replacing conventional battery-dependent power sources with ambient mechanical energy harvesters, and it evaluates the relative merits of inorganic ceramics, organic polymers, and composite systems in achieving efficient electromechanical conversion under practical operating conditions. The discussion further considers compositional tuning, phase boundary engineering, microstructural optimization, and device-level integration as key strategies for improving piezoelectric output, mechanical compliance, durability, and manufacturability. By connecting fundamental materials design with application-driven device requirements, the review identifies the principal challenges and emerging directions necessary for the realization of reliable, scalable, and sustainable electronic platforms.

The expansion of smart healthcare and wearable electronics has intensified the need for fabric-based sensors that integrate conformally with the human body for continuous bio signal monitoring. However, the heavy reliance of conventional devices on external batteries remains a major obstacle to commercialization, necessitating the development of flexible piezoelectric energy harvesters that convert biomechanical energy into sustainable power. Here, we present a highly flexible and wearable piezoelectric energy harvester (PEH) fabricated by a screen-printing of BaTiO₃ nanoparticlePDMS composites onto a fabric substrate. An optimized piezo-ceramic filler concentration of 70 wt% yielded a peak output voltage of 0.52 V and a current of 40 nA under the mechanical bending deformations. The fabricated PEH demonstrated exceptional mechanical and electrical stability, showing no performance degradation of over 5,000 repetitive bending cycles. These results indicate that a PEH can function as a stable self-powered source within complex clothing environments, offering a promising pathway for next-generation autonomous wearable sensor systems.

Bismuth layer-structured ferroelectrics with high Curie temperatures have recently attracted significant attention as promising candidates for high-temperature piezoelectric applications. However, the conventional solid-state reaction method entails high-temperature processing that induces bismuth volatilization, thereby degrading device reliability. In this study, we employed a co-precipitation method enabling atomic-level mixing to significantly lower the synthesis temperature of Nb/Tadoped Bi₄Ti₃O₁₂ ceramics compared to the solid-state reaction method. Experimental results demonstrated that the coprecipitation method yielded a pure single phase at 600℃ without intermediate phases. Furthermore, the synthesized nanopowders, with an average size of 100 nm, lowered the onset temperature of sintering shrinkage to 650℃, approximately 200℃ lower than that of the solid-state counterpart. The low-temperature synthesis process proposed in this work is expected to contribute to the performance enhancement of high-temperature piezoelectric devices by effectively suppressing bismuth volatilization and ensuring compositional stability.

The rapid evolution of wearable technology has driven a surge in demand for sustainable, self-powered electronic devices. Flexible thermoelectric materials, capable of converting body heat into electricity, have emerged as a promising solution for powering next-generation wearables. This review comprehensively examines recent progress in organic (polymer-based) and hybrid thermoelectric materials, focusing on their design, fabrication, and integration into flexible architectures suitable for conformal contact with human skin. Key developments include advanced doping strategies, post-treatment techniques, and composite engineering, particularly in conductive polymers such as PEDOT: PSS and P3HT, which have significantly enhanced power factors and mechanical flexibility. Additionally, the integration of high-performance inorganic materials into stretchable systems has further elevated device efficiency and durability. The review highlights breakthroughs, ongoing challenges, and future opportunities in realizing practical, scalable, and high-efficiency wearable thermoelectric generators for sustainable energy harvesting applications.

Citations

• Design and optimization of all-segmented thermoelectric legs based on Bi2Te3 and SnTe for wide-range energy harvesting
  Hyejeong Choi, Momanyi Amos Okirigiti, Nagamalleswara Rao Alluri, Jong Min Park, Donghyun Shin, Ho Seong Lee, Kyung Tae Kim, Changyeon Baek, Min-Ku Lee, Gyoung-Ja Lee, Kwi-Il Park
  Journal of Power Sources.2026; 691: 240981.     CrossRef

The continuous and long-lasting monitoring of physiological signals induced from the human body is crucial for health monitoring, disease diagnosis, and treatment. In this study, we have reported the Seebeck effect-based flexible selfpowered temperature sensor which can convert the electric signals from lateral temperature difference. For demonstrating temperature sensor arrays, the p-type thermoelectric (TE) composite films were fabricated by dispersing the Bi_0.5Sb_1.5Te₃ (BST) powders inside poly-vinylidene fluoride matrix and subsequently attached to the patterned electrode foils. The inorganic BST powders-embedded TE composite films with activated area of 0.5 × 1 cm² harvest a maximum voltage of 1.7 mV, a maximum current of 5.6 mA, and an output power of 2.6 nW from the temperature gradient (ΔT) of 20 K. Finally, the fabricated selfpowered temperature sensor array well detected the pattern images of external thermal source of ΔT = 20 K. This study manifests flexible temperature sensor array which paves the way for further advancements in this field.

Conductive inks are essential for developing flexible and wearable electronic devices, where printability and electrical performance must be finely balanced. However, achieving high conductivity while minimizing costly silver filler content remains a key challenge in ink formulation. In this work, we demonstrate that a simple ball-milling process transforms spherical silver particles into platelet-shaped fillers, dramatically enhancing conductivity at equivalent filler loading. The resulting inks show a reduction in sheet resistance from ~180 Ω/□ to ~ 0.57 Ω/□ at 70 wt% filler content, with improved performance attributed to surface-to-surface contact between platelets. Moreover, we show that filler content influences not only electrical conductivity but also ink viscosity, with the 53.8 wt% formulation achieving a practical balance between conductivity, processability, and cost. This morphology- and composition-controlled ink design offers a scalable strategy for manufacturing high-performance, cost-effective conductive inks suitable for next-generation printed electronics.

The polymer crystallization process, promoting the formation of ferroelectric β-phase, is essential for developing polyvinylidene fluoride (PVDF)-based high-performance piezoelectric energy harvesters. However, traditional high-temperature annealing is unsuitable for the manufacture of flexible piezoelectric devices due to the thermal damage to plastic components that occurs during the long processing times. In this study, we investigated the feasibility of introducing a flash lamp annealing that can rapidly induce the β-phase in the PVDF layer while avoiding device damage through selective heating. The flash lightirradiated PVDF films achieved a maximum β-phase content of 76.52% under an applied voltage of 300 V and an on-time of 1.5 ms, a higher fraction than that obtained through thermal annealing. The PVDF-based piezoelectric energy harvester with the optimized irradiation condition generates a stable output voltage of 0.23 V and a current of 102 nA under repeated bendings. These results demonstrate that flash lamp annealing can be an effective process for realizing the mass production of PVDF-based flexible electronics.

Citations

• In Situ Amidation‐Derived Interfacial Modulation for Homogeneous Ultra‐High Nanoparticle Loading Toward Robust and Flexible Piezoelectric Composites
  HakSu Jang, In Beom Heo, Changyeon Baek, Dong Won Jeon, Donghun Lee, Nagamalleswara Rao Alluri, Hyejeong Choi, HyoMin Jeon, SungHoon Kim, Hyunseung Kim, Jihun Choi, Hyun‐Soo Chang, Chang Kyu Jeong, Min‐Ku Lee, Jun Mo Koo, Tiandong Zhang, Geon‐Tae Hwang, S
  Advanced Functional Materials.2026;[Epub]     CrossRef

Laser-induced plasmonic sintering of metal nanoparticles (NPs) holds significant promise as a technology for producing flexible conducting electrodes. This method offers immediate, straightforward, and scalable manufacturing approaches, eliminating the need for expensive facilities and intricate processes. Nevertheless, the metal NPs come at a high cost due to the intricate synthesis procedures required to ensure long-term reliability in terms of chemical stability and the prevention of NP aggregation. Herein, we induced the self-generation of metal nanoparticles from Ag organometallic ink, and fabricated highly conductive electrodes on flexible substrates through laser-assisted plasmonic annealing. To demonstrate the practicality of the fabricated flexible electrode, it was configured in a mesh pattern, realizing multi-touchable flexible touch screen panel.

Citations

• Controlling Structures and Properties of NaCl‐Containing Alginate/Polyacrylamide Tough Hydrogels via a One‐Pot Process
  Taeuk Eom, Hyunseung Kim, Jihun Choi, Soon Joo Yoon, Yoon Kyeung Lee, Kwi‐Il Park, Chang Kyu Jeong
  Chemistry – A European Journal.2026;[Epub]     CrossRef
• Wearable sweat glucose monitoring patches enabled by double network hydrogel-MoS2/PEDOT: PSS nanocomposite
  Suraj Shinde, Omkar A. Patil, Sang Yoon Park, Se Jin Choi, Omkar Pawar, Daniel J. Joe, Sooman Lim, Han Eol Lee
  Microchemical Journal.2025; 215: 114309.     CrossRef

Flash lamp annealing (FLA) of metal nanoparticle (NP) ink has provided powerful strategies to fabricate highperformance electrodes on a flexible substrate because of its rapid processing capability (in milliseconds), low-temperature process, and compatibility with to roll-to-roll process. However, metal NPs [e.g., gold (Au), silver (Ag), copper (Cu), etc.] have limitations such as difficulty in synthesizing fine metal NPs (diameter less than 10 nm), high price, and degradation during ink storage and FLA processing. In this regard, organometallic ink has been proposed as a material that can replace metal NPs due to their low-cost (usually 1/100 times cheaper than metal nano inks), low-temperature processability, and high material stability. Despite these advantages, the fabrication of flexible electrodes through FLA treatment of organometallic compounds has not been extensively researched. In this paper, we experimentally guide how to determine the optimal conditions for forming electrodes on flexible substrates by considering material parameters, and flashlight processing parameters (energy density, pulse duration, etc) to minimize the difficulties that may arise during the FLA of organometallic ink.

Stretchable piezoelectric energy harvester (S-PEHs) based on composite materials are considered one of the potential candidates for realizing wearable self-powered devices for smart clothing and electronic skin. However, low energy conversion performance and expensive stretchable electrodes are major bottlenecks hindering the development and application of S-PEHs. Here, we fabricated the S-PEH by adopting the piezoelectric composites with enhanced stress transfer properties and kirigamipatterned textile electrodes. The optimum contents of piezoelectric BaTiO₃ nanoparticles inside the carbon nanotube/ecoflex composite were selected as 30 wt% considering the trade-off between stretchability and energy harvesting performance of the device. The final S-PEH shows an output voltage and mechanical stability of ~5 V and ~3,000 cycles under repeated 150% of tensile strain, respectively. This work presents a cost-effective and scalable way to fabricate stretchable piezoelectric devices for self-powered wearable electronic systems.

Citations

• Long‐Lasting, Steady and Enhanced Energy Harvesting by Inserting a Conductive Layer into the Piezoelectric Polymer
  HakSu Jang, Gwang Hyeon Kim, Dong Won Jeon, Hyeon Jun Park, BitNa Bae, Nagamalleswara Rao Alluri, Cheol Min Kim, Changyeon Baek, Min‐Ku Lee, Sung Beom Cho, Gyoung‐Ja Lee, Kwi‐Il Park
  Advanced Functional Materials.2025;[Epub]     CrossRef

Recent advancement of Internet of Things (IoT) and energy harvesting technology enable realization of flexible thermoelectric energy harvester (f-TEH), with technological prowess for use in biomedical monitoring system integrated applications. To expand a flexible thermoelectric energy harvesting platform, the f-TEH must be required for optimized flexible thermoelectric materials and device structure. In response to these demands related to thermoelectric energy harvesting, many research groups have investigated various f-TEHs applied as a power source for wearable electronics. As a key member of the f-TEH, film-based f-TEHs possess significant applicability in research to realize self-powered wearable electronics, owing to their excellent flexibility, low thermal conductivity, and convenient fabrication process. Thus, based on the rapid growth of thermoelectric film technology, this review aims to overview comprehensively the f-TEH made of various inorganic/organic thermoelectric materials including developed fabrication methods, high thermoelectric performance, and wide-range applications.

Piezoelectric energy harvesting technologies, which can be used to convert the electricity from the mechanical energy, have been developed in order to assist or power the wearable electronics. To realize non-toxic and biocompatible electronics, the lead-free (Ba_0.85Ca_0.15)(Ti_0.90Zr_0.10)O₃ (BCTZ) nanoparticles (NPs) are being studied with a great attention as flexible energy harvesting device. Herein, piezoelectric hybrid nanocomposites were fabricated using BCTZ NPs-embedded poly(vinylidene fluoride-trifluoroethylene) [P(VDF-TrFE)] matrix to improve the performance of flexible energy harvester. Output performance of the fabricated energy device was investigated by the well-optimized measurement system during the periodically bending and releasing motions. The generated open-circuit voltage and the short-circuit current of the piezoelectric hybrid nanocomposite-based energy harvester reached up to ~15 V and ~1.1 μA, respectively; moreover, the instantaneous power of 3.5 μW is determined from load voltage and current at the external load of 20 MΩ. This research is expected to cultivate a new approach to high-performance wearable self-powering electronics.