Flexible Thermoelectric Devices Research Articles

Layer by layer flexible organic thermoelectric devices based on PEDOT:PSS and PBFDO

Layer by layer flexible organic thermoelectric devices based on PEDOT:PSS and PBFDO

High-performance flexible p-type Ce-filled Fe3CoSb12 skutterudite thin film for medium-to-high-temperature applications

P-type Fe3CoSb12-based skutterudite thin films are successfully fabricated, exhibiting high thermoelectric performance, stability, and flexibility at medium-to-high temperatures, based on preparing custom target materials and employing advanced pulsed laser deposition techniques to address the bonding challenge between the thin films and high-temperature flexible polyimide substrates. Through the optimization of fabrication processing and nominal doping concentration of Ce, the thin films show a power factor of >100 μW m−1 K−2 and a ZT close to 0.6 at 653 K. After >2000 bending cycle tests at a radius of 4 mm, only a 6 % change in resistivity can be observed. Additionally, the assembled p-type Fe3CoSb12-based flexible device exhibits a power density of 135.7 µW cm−2 under a temperature difference of 100 K with the hot side at 623 K. This work fills a gap in the realization of flexible thermoelectric devices in the medium-to-high-temperature range and holds significant practical application value.

Flexible Thermoelectric Device Based on Protrusion-Structured Liquid Metal Elastomer for Gravity Heat Pipe.

Monitoring the temperature of the coal gangue mountains is fundamental to preventing their spontaneous combustion. However, the existing temperature monitoring systems fail to achieve stable, pollution-free temperature monitoring without affecting vegetation growth in these mountains. To address this issue, this work proposes a flexible thermoelectric device (FTD) based on a protrusion-structured liquid metal elastomer (LME). Utilizing a high-thermal-conductivity LME, the FTD adheres closely to the surface of the gravity heat pipe (GHP), ensuring compatibility between FTD and the curved surface of the GHP. Simultaneously, employing a low-thermal-conductivity elastomer helps concentrate heat onto FTD, thereby enhancing thermoelectric power generation efficiency. Additionally, the impact of the shape, size, and height of the protrusion structure at the cold end of the GHP on its efficiency was also investigated. The practical application of FTD on GHP was demonstrated.

High‐Performance Self‐Powered Flexible Thermoelectric Device for Accelerated Wound Healing

AbstractElectric signal accelerates full‐thickness wound healing in the clinic, which is usually generated by a large power generation system and requires delicate control by authorized personnel. Here, a self‐powered flexible and biocompatible thermoelectric device with exceptionally high power generation efficiency is developed. It generates 10 mV voltage at a temperature gradient of 10 K, outperforming all reported flexible thermoelectric devices. Accordingly, it can directly and efficiently convert the omnipresent heat in the skin to electricity at the microvolt level. The output electricity activates and upregulates the expression of Piezo1‐mediated pathways that are associated with tissue regeneration, accelerating the cell migration and proliferation in vitro and healing the wound 4 days faster in vivo. Importantly, the thermoelectric device fast‐heals the wound without involving any additional electric circuit such as an amplifier. These advantages will revolutionize the designing of self‐powered wearable bioelectronics for diagnosing, monitoring, and treating various pathological conditions employing the skin heat.

Transparent and flexible thermoelectric thin films based on copper sulfides

As a promising thermoelectric material, CuS has attracted significant attention due to its high conductivity, abundance of elements, and eco-friendliness. However, the study on CuS-based thermoelectric thin films is still lacking, impeding the advancement of CuS-based thermoelectric devices. Herein, high-quality CuS thin films have been fabricated through a facile vulcanization process. The effects of vulcanization temperature and film thickness on the thermoelectric properties of CuS thin films have been investigated. An optimal high power factor of 73.25 μW/m−1 K−2 is found at 400 K for a 20 nm-thick sample, and the optical transmittance is over 80% in the visible light spectrum. Meanwhile, excellent flexibility of the CuS thin films has been demonstrated. These results demonstrate the high promise of CuS thin films for transparent and flexible thermoelectric device applications.

Metallic barrier layer for Ag2S1−xSex inorganic ductile thermoelectric materials

Metallic barrier layer is a key component in thermoelectric (TE) devices, but it is rarely investigated for the recently discovered inorganic ductile TE materials. In this work, we demonstrate that tungsten (W) is the excellent metallic barrier layer for Ag2S1−xSex ductile thermoelectric materials. The phase composition, microstructure, adhesive strength, and interfacial contact resistivity (ρC) of the W/Ag2S1−xSex joint have been systematically investigated. The sputtered W film has high adhesive strength and little interdiffusion/reaction with Ag2S1−xSex. The ρC decreases with increasing the Se content, which can be understood by the Thermionic-field Emission model. This work would guide the development of high-performance flexible TE devices based on ductile TE materials.

The Enhanced Thermoelectric and Mechanical Performance of Polythiophene/Single-Walled Carbon Nanotube Composites with Polar Ethylene Glycol Branched-Chain Modifications.

In order to develop flexible thermoelectric materials with thermoelectric and mechanical properties, in this study, we designed and synthesized polythiophene derivatives with branched ethylene glycol polar side-chains named P3MBTEMT, which were used in combination with single-walled carbon nanotubes (SWCNTs) to prepare composite thin films and flexible thermoelectric devices. A comparison was made with a polymer named P3(TEG)T, which has a polar alkoxy linear chain. The UV-vis results indicated that the larger steric hindrances of the branched ethylene glycol side-chain in P3MBTEMT could inhibit its self-aggregation and had a stronger interaction with the SWCNTs compared to that of P3(TEG)T, which was also confirmed using Raman spectroscopy. When the mass ratio of SWCNTs to P3MBTEMT was 9:1 (represented as P3MBTEMT/SWCNTs-0.9), the composite film exhibited the highest thermoelectric properties with a power factor of 446.98 μW m-1 K-2, which was more than two times higher than that of P3(TEG)T/SWCNTs-0.9 (215.08 μW m-1 K-2). The output power of the thermoelectric device with P3MBTEMT/SWCNTs-0.9 was 2483.92 nW at 50 K, which was 1.66 times higher than that of P3(TEG)T/SWCNTs-0.9 (1492.65 nW). Furthermore, the P3MBTEMT/SWCNTs-0.5 showed superior mechanical properties compared to P3(TEG)T/SWCNTs-0.5. These results indicated that the mechanical and thermoelectric performances of polymer/SWCNT composites could be significantly improved by adding polar branched side-chains to conjugated polymers. This study provided a new strategy for creating high-performing novel flexible thermoelectric materials.

Synthesis, Characterization and Power Factor Estimation of SnSe Thin Film for Energy Harvesting Applications

In this work, a simple, cost-effective successive ionic layer adsorption and reaction (SILAR) deposition technique has been used to deposit a high-quality tin selenide (SnSe) thin film onto a glass substrate. Structural, morphologic, and thermoelectric properties have been characterized for the prepared thin film. X-ray diffraction (XRD) results of the SnSe thin film reveal an orthorhombic structure phase. The morphological properties of the prepared thin films have been studied using field emission scanning electron microscopy (FESEM). The stoichiometric composition of the deposited thin film and the elemental binding energies of the Sn and Se elements have been investigated with energy-dispersive spectroscopy (EDS) and X-ray photoelectron spectroscopy (XPS). The Fourier transformation infrared (FTIR) spectrum of the SnSe thin film displays vibrational modes of chalcogenides bonds. These results suggest that the developed thin film is crystalline, uniform, and without impurities and is appropriate for energy harvesting applications. The prepared thin film’s Seebeck coefficient and electrical resistivity were estimated through ZEM-3 from room temperature to 600 K. The power factor was evaluated. A substantially high electrical conductivity is observed, which decreases somewhat with temperature, suggesting a semimetal conducting transport—the absolute values of the Seebeck coefficient increase with temperature. The resulting power factor showed the highest values near room temperature and a somewhat decreasing trend as the temperature increased. Despite lower values of the Seebeck coefficient, the substantially enhanced power factor is due to the higher electrical conductivity of the thin film, superior to that reported previously. This precursor study demonstrates promising results for developing high-performance flexible thermoelectric devices via a simple and facile SILAR strategy.

Manipulating Hetero-Nanowire Films for Flexible and Multifunctional Thermoelectric Devices.

Flexible thermoelectric devices hold significant promise in wearable electronics owing to their capacity for green energy generation, temperature sensing, and comfortable wear. However, the simultaneous achievement of excellent multifunctional sensing and power generation poses a challenge in these devices. Here, ordered tellurium-based hetero-nanowire films are designed for flexible and multifunctional thermoelectric devices by optimizing the Seebeck coefficient and power factor. The obtained devices can efficiently detect both object and environment temperature, thermal conductivity, heat proximity, and airflow. In addition, combining the thermoelectric units with radiative cooling materials exhibits remarkable thermal management capabilities, preventing device overheating and avoiding degradation in power generation. Impressively, this multifunctional electronics exhibits excellent resistance in extreme low earth orbit environments. The fabrication of such thermoelectric devices provides innovative insights into multimodal sensing and energy harvesting.

Effects of Ag off-stoichiometry on mechanical and thermoelectric properties of ductile AgCuSe0.6S0.4

Recently, AgCuSe-based ductile inorganic thermoelectric (TE) materials have attracted great interests because they can simultaneously achieve excellent TE performance and good deformability at room temperature. The composition-performance relationship of p-type AgCuSe-based ductile inorganic TE materials have been systematically investigated, but the related investigation on n-type AgCuSe-based ductile inorganic TE materials is still absent. In this work, a series of n-type ductile Ag1+xCuSe0.6S0.4 (x = −0.02, −0.01, 0, 0.01, and 0.02) samples are prepared. The effects of Ag off-stoichiometry on the phase composition, mechanical, and TE properties are systematically investigated. The crystal structure of AgCuSe0.6S0.4 can accommodate a small amount of Ag-excess to maintain the phase purity, but very little Ag-deficiency can induce the formation of secondary phases. The Ag off-stoichiometry has little influence on the mechanical performance. Introducing Ag-excess can increase the carrier concentration to optimize the electrical conductivity and power factor, leading to enhanced TE figure-of-merit (zT). The zT of Ag1.02CuSe0.6S0.4 is 0.17 at 300 K. The six-couple in-plane flexible TE device fabricated based on Ag1.02CuSe0.6S0.4 demonstrates high output performance that is superior to the organic flexible TE devices. This work deepens the understanding on the novel AgCuSe-based ductile inorganic TE materials.

N-DMBI Doping of Carbon Nanotube Yarns for Achieving High n-Type Thermoelectric Power Factor and Figure of Merit.

The application of carbon nanotube (CNT) yarns as thermoelectric materials for harvesting energy from low-grade waste heat including that generated by the human body, is attracting considerable attention. However, the lack of efficient n-type CNT yarns hinders their practical implementation in thermoelectric devices. This study reports efficient n-doping of CNT yarns, employing 4-(1, 3-dimethyl-2, 3-dihydro-1H-benzimidazole-2-yl) phenyl) dimethylamine (N-DMBI) in alternative to conventional n-dopants, with o-dichlorobenzene emerging as the optimal solvent. The small molecular size of N-DMBI enables highly efficient doping within a remarkably short duration (10s) while ensuring prolonged stability in air and at high temperature (150°C). Furthermore, Joule annealing of the yarns significantly improves the n-doping efficiency. Consequently, thermoelectric power factors (PFs) of 2800, 2390, and 1534µWm-1 K-2 are achieved at 200, 150, and 30°C, respectively. The intercalation of N-DMBI molecules significantly suppresses the thermal conductivity, resulting in the high figure of merit (ZT) of 1.69×10-2 at 100°C. Additionally, a π-type thermoelectric module is successfully demonstrated incorporating both p- and n-doped CNT yarns. This study offers an efficient doping strategy for achieving CNT yarns with high thermoelectric performance, contributing to the realization of lightweight and mechanically flexible CNT-based thermoelectric devices.

Vertically designed high-performance and flexible thermoelectric generator based on optimized PEDOT:PSS/SWCNTs composite films

To solve the long-lasting challenge of low thermoelectric performance of flexible thermoelectric device (F-TEG), in this work, we report a three-dimensional vertically structured F-TEG composed of flexible, stable, and high-performing p- and n-type single-walled carbon nanotube (SWCNT)-based composite films. The p-type SWCNT-based composite film exhibits a high room-temperature power factor of >500 μW m−1 K−2, benefiting from the effective de-doping of the hybridized poly(3,4-ethylenedioxythiophene)–poly(styrenesulfonate) (PEDOT:PSS) using a binary co-doping agent composed of NaHCO3 and the polar solvent ethylene glycol (EG). Simultaneously, the n-type SWCNT-based film doped with the amine-rich electron donor polyethyleneimine (PEI) is prepared, exhibiting a high room-temperature power factor of 185.4 μW m−1 K−2 and excellent air stability. By employing flexible supporting foam, vertical p-n thermoelectric legs are realized, and the F-TEG based on these legs exhibits a maximum open-circuit voltage of 23.2 mV and a maximum output power of 2.6 μW at a temperature difference of 48 K, demonstrating a competitive normalized power density of >2.5 μW cm−2 K−2, which advances the low-power flexible wearable field.

Fully inkjet-printed Ag2Se flexible thermoelectric devices for sustainable power generation

Flexible thermoelectric devices show great promise as sustainable power units for the exponentially increasing self-powered wearable electronics and ultra-widely distributed wireless sensor networks. While exciting proof-of-concept demonstrations have been reported, their large-scale implementation is impeded by unsatisfactory device performance and costly device fabrication techniques. Here, we develop Ag2Se-based thermoelectric films and flexible devices via inkjet printing. Large-area patterned arrays with microscale resolution are obtained in a dimensionally controlled manner by manipulating ink formulations and tuning printing parameters. Printed Ag2Se-based films exhibit (00 l)-textured feature, and an exceptional power factor (1097 μWm−1K−2 at 377 K) is obtained by engineering the film composition and microstructure. Benefiting from high-resolution device integration, fully inkjet-printed Ag2Se-based flexible devices achieve a record-high normalized power (2 µWK−2cm−2) and superior flexibility. Diverse application scenarios are offered by inkjet-printed devices, such as continuous power generation by harvesting thermal energy from the environment or human bodies. Our strategy demonstrates the potential to revolutionize the design and manufacture of multi-scale and complex flexible thermoelectric devices while reducing costs, enabling them to be integrated into emerging electronic systems as sustainable power sources.

High efficient personal thermoregulatory device: Metallized interface layer between flexible polyimide substrate and foam copper heat sink enables thermal resistance reduction

Customizable flexible thermoelectric devices (f-TED) designed for personal thermal management (PTM) have the potential to substantially diminish energy consumption while enhancing comfort. Currently, studies focus on optimizing thermoelectric device performance and reducing radiator thermal resistance, neglecting the crucial interface between them. In this innovative work, the interface layer between the flexible polyimide substrate of f-TED and the foam copper heat sink was metallized, thereby significantly mitigating the thermal resistance at the interface. In contrast to the conventional thermal conductive adhesive, the metallized welding thermoelectric system (4 × 4 cm² in the plane) demonstrates a 37.0 % augmentation in cooling temperature difference (5.4 ℃ → 7.4 ℃) at 0.3 A. When bending 1000 times (r: ∞ → 20 mm → ∞ → …), the change rate of internal resistance is less than 1.5 %. At a temperature difference of 20 K, it reaches a maximum output power as high as 4.45 mW. Furthermore, an intelligent personal thermal management system was developed. Users can monitor and adjust the working status of the f-TED in real-time via a mobile terminal, achieving personalized thermoregulation. In actual human wear tests, the highest cooling temperature difference reached 13.7 °C, which is one of the highest reported values. This work holds significant implications for advancing f-TED technology innovation, personalized thermoregulation, energy conservation, and environmental protection.

Hydraulic-driven adaptable morphing active-cooling elastomer with bioinspired bicontinuous phases

The active-cooling elastomer concept, originating from vascular thermoregulation for soft biological tissue, is expected to develop an effective heat dissipation method for human skin, flexible electronics, and soft robots due to the desired interface mechanical compliance. However, its low thermal conduction and poor adaptation limit its cooling effects. Inspired by the bone structure, this work reports a simple yet versatile method of fabricating arbitrary-geometry liquid metal skeleton-based elastomer with bicontinuous Gyroid-shaped phases, exhibiting high thermal conductivity (up to 27.1 W/mK) and stretchability (strain limit >600%). Enlightened by the vasodilation principle for blood flow regulation, we also establish a hydraulic-driven conformal morphing strategy for better thermoregulation by modulating the hydraulic pressure of channels to adapt the complicated shape with large surface roughness (even a concave body). The liquid metal active-cooling elastomer, integrated with the flexible thermoelectric device, is demonstrated with various applications in the soft gripper, thermal-energy harvesting, and head thermoregulation.

Chemically Transformed Ag2 Te Nanowires on Polyvinylidene Fluoride Membrane For Flexible Thermoelectric Applications.

Flexible thermoelectric devices of nanomaterials have shown a great potential for applications in wearable to remotely located electronics with desired shapes and geometries. Continuous powering up the low power flexible electronics is a major challenge. We are reporting a flexible thermoelectric module prepared from silver telluride (Ag2 Te) nanowires (NWs), which are chemically transformed from uniquely synthesized and scalable tellurium (Te) NWs. Conducting Ag2 Te NWs composites have shown an ultralow total thermal conductivity ~0.22 W/mK surpassing the bulk melt-grown Ag2 Te ~1.23 W/mK at ~300 K, which is attributed to the nanostructuring of the material. Flexible thermoelectric device consisting of 4 legs (n-type) of Ag2 Te NWs on polyvinylidene fluoride membrane displays a significant output voltage (Voc ) ~2.3 mV upon human touch and Voc ~18 mV at temperature gradient, ΔT ~50 K, which shows the importance of NWs based flexible thermoelectric devices to power up the low power wearable electronics.

Chemically Transformed Ag2Te Nanowires on Polyvinylidene Fluoride Membrane For Flexible Thermoelectric Applications

AbstractFlexible thermoelectric devices of nanomaterials have shown a great potential for applications in wearable to remotely located electronics with desired shapes and geometries. Continuous powering up the low power flexible electronics is a major challenge. We are reporting a flexible thermoelectric module prepared from silver telluride (Ag2Te) nanowires (NWs), which are chemically transformed from uniquely synthesized and scalable tellurium (Te) NWs. Conducting Ag2Te NWs composites have shown an ultralow total thermal conductivity ~0.22 W/mK surpassing the bulk melt‐grown Ag2Te ~1.23 W/mK at ~300 K, which is attributed to the nanostructuring of the material. Flexible thermoelectric device consisting of 4 legs (n‐type) of Ag2Te NWs on polyvinylidene fluoride membrane displays a significant output voltage (Voc) ~2.3 mV upon human touch and Voc ~18 mV at temperature gradient, ΔT ~50 K, which shows the importance of NWs based flexible thermoelectric devices to power up the low power wearable electronics.

Flexible power generators by Ag2Se thin films with record-high thermoelectric performance

Exploring new near-room-temperature thermoelectric materials is significant for replacing current high-cost Bi2Te3. This study highlights the potential of Ag2Se for wearable thermoelectric electronics, addressing the trade-off between performance and flexibility. A record-high ZT of 1.27 at 363 K is achieved in Ag2Se-based thin films with 3.2 at.% Te doping on Se sites, realized by a new concept of doping-induced orientation engineering. We reveal that Te-doping enhances film uniformity and (00l)-orientation and in turn carrier mobility by reducing the (00l) formation energy, confirmed by solid computational and experimental evidence. The doping simultaneously widens the bandgap, resulting in improved Seebeck coefficients and high power factors, and introduces TeSe point defects to effectively reduce the lattice thermal conductivity. A protective organic-polymer-based composite layer enhances film flexibility, and a rationally designed flexible thermoelectric device achieves an output power density of 1.5 mW cm−2 for wearable power generation under a 20 K temperature difference.

Pulse irradiation synthesis of metal chalcogenides on flexible substrates for enhanced photothermoelectric performance

High synthesis temperatures and specific growth substrates are typically required to obtain crystalline or oriented inorganic functional thin films, posing a significant challenge for their utilization in large-scale, low-cost (opto-)electronic applications on conventional flexible substrates. Here, we explore a pulse irradiation synthesis (PIS) to prepare thermoelectric metal chalcogenide (e.g., Bi2Se3, SnSe2, and Bi2Te3) films on multiple polymeric substrates. The self-propagating combustion process enables PIS to achieve a synthesis temperature as low as 150 °C, with an ultrafast reaction completed within one second. Beyond the photothermoelectric (PTE) property, the thermal coupling between polymeric substrates and bismuth selenide films is also examined to enhance the PTE performance, resulting in a responsivity of 71.9 V/W and a response time of less than 50 ms at 1550 nm, surpassing most of its counterparts. This PIS platform offers a promising route for realizing flexible PTE or thermoelectric devices in an energy-, time-, and cost-efficient manner.

High-performance flexible thermoelectric devices with a copper foam heatsink for personal thermal management

A Bi2Te3-based thermoelectric device with high thermoelectric performance and flexibility for human body waste heat recovery and temperature management.