Thermoelectric Legs Research Articles

Enhancing the Thermoelectric Performance of n-Type Mg3Sb2-Based Materials via Ag Doping.

The n-type Mg3(Sb, Bi)2 compounds show great potential for wasted heat energy harvesting due to their promising thermoelectric properties. This work discovers that doping transition element Ag into the n-type Mg3(Sb, Bi)2 can effectively optimize the power factor and suppress the lattice thermal conductivity simultaneously. Interestingly, the Ag doping has different effects compared to the isoelectronic and same group element Cu addition studied previously. A high power factor of 19.6µW cm-1 K-2 is obtained at 673K owing to the increased electrical conductivity. At the same time, the lattice thermal conductivity is reduced to ≈0.5W m-1 K-1 because of enhanced phonon scattering induced by Ag atoms. These improvements lead to a peak figure of merit (ZT) of 1.64 at 673K as well as a high average ZT of 1.27 is obtained from 323 K to 673K. Furthermore, a thermoelectric single leg with a competitive conversion efficiency of ≈11% under a hot-side temperature of 673K is fabricated successfully. In addition, a 2-pair module composed of n-type Mg3(Sb, Bi)2 alloy and p-type MgAgSb-based compound demonstrates the high conversion efficiency of ≈7.9% at a temperature difference of 277K, which will significantly upgrade the sustainable energy recycling technology.

Thermally induced vibration of photovoltaic honeycomb-based-thermoelectric hybrid device

This paper presents a comprehensive investigation of thermally induced vibration (TIV) of elastically constrained photovoltaic honeycomb-based-thermoelectric hybrid device under space thermal environment. Based on four-variable refined quasi-3D higher-order theory as well as virtual boundary spring technique, the equation of motion of the hybrid device is derived by using Lagrange equation. The nonlinear temperature profile is obtained via finite difference scheme and the TIV responses are solved by employing Newmark approach. The effects of boundary condition, size of honeycomb cell, damping effect, thickness of insulation layer and radius of curvature on TIV of the hybrid device are studied. Results show that the TIV response of the hybrid device can be greatly weakened by replacing the dense thermoelectric leg with honeycomb-based thermoelectric leg. Designing the honeycomb cell as re-entrant architecture possesses a better suppression effect on TIV response. The amplitude of TIV reduces with increasing the thickness-length ratio and decreasing the height-length ratio of honeycomb cell. A larger thickness of insulation layer can weaken the TIV response. The oscillation of TIV response can be eliminated by fabricating hybrid device as circular cylindrical and hyperbolic parabolic shallow shells. The stiffer the boundary conditions, the less prone to TIV behavior of the hybrid device. The introduction of damping effect can suppress TIV response, but it simultaneously causes the occurrence of thermal snap. In general, the research provides several design references to weaken the TIV response of the hybrid device under space heat flux.

Influence of Hydration and Temperature on the NaxCO2 Based Transducer Voltage

This paper presents an experimental approach to maximizing the voltage generated by NaxCoO2 and improving the overall efficiency of the p-type thermoelectric leg by doping with Na up to x = 0.88. Two samples with different geometries were tested, each measured with and without an additional magnetic field applied in the direction of the temperature gradient. The properties of sodium cobaltite in response to hydration were explored, at temperatures between 300 and 380 K. Water injection boosted the current and power up to 75–100 µW at a temperature of 350–360 K. This power boost can be attributed to an electron-ion fluid flow pattern maintained by the longitudinal thermomagnetic effect and by water molecules forming hydrogen bonds with oxygen atoms in the CoO2 layers, inside the material. An electronic circuit was designed to boost the voltage to the desired level, for three or more sodium cobaltite samples mounted in parallel, and to store the energy in a supercapacitor. The output voltage and resistivity change of sodium cobaltite samples can be readily used as a humidity and temperature-sensing element in a transducer when paired with an appropriate electronic conditioning scheme.

Integrating dual heat sources to enhance thermoelectric generator power output

The escalating demand for sustainable power sources for wearable electronics necessitates innovative solutions. This study tackles the challenge of sustainably powering wearable electronics, addressing the limitations of traditional batteries. The approach utilizes a thermoelectric generator with a flexible and stretchable substrate that integrates the photothermal effect and human body temperature as a heat source. A unique strategy is employed to achieve this, involving the combination of 10 g of polydimethylsiloxane, 0.5 g of carbon nanotubes powder, 1 g of base curing agent, and 1.15 g of ethyl acetate mixture used as the novel substrate material. The proposed composite substrate is paired with p-type and n-type thermoelectric legs of bismuth antimony telluride (Bi0.4Sb1.6Te3) and bismuth selenium telluride (Bi1.7Te3.7Se0.3), respectively. This innovative design ensures high flexibility, stretchability, and conformability, facilitating seamless integration into wearable electronic devices. Experimental validation and simulation-based studies reveal a power density of 166.29 μW/cm2, sufficient for powering small-scale wearable electronics. The thermoelectric generator coupled with a novel composite substrate showed 65.6 % stretchability, further underscoring its durability and adaptability. The critical finding lies in the dual heat source integration, which collectively boosts power output and ensures year-round performance, pushing the boundaries of wearable energy harvesting technologies.

Elaboration of p-type Ge doped MnSiy (1.73 < y < 1.77) thermoelectric legs with complex shapes by binder jetting additive manufacturing technique

Thermoelectric legs with complex geometries exhibit high potential interest for fatal heat conversion into electricity due to higher thermal dissipation. Additive manufacturing (AM)is a solution of choice to decrease the manufacturing cost of thermoelectric legs that are historically requiring lengthy and costly fabrication processes and it gives the possibility of custom legs geometry. Nevertheless, microcracks and high porosity are commonly present by using this kind of process for thermoelectric materials leading to by limited performances. This work reports the possibility to manufacture n type Ge doped MnSiy (1.73 < y < 1.77) thermoelectric legs with various shapes without microcracks and with low porosity using the binder jetting AM technique followed by a Spark Plasma Sintering (SPS) step. The Mn15Si26 phase in the samples is systematically present, the samples density can reach 98%. A power factor of 1130 µW.m-1K-2 was reached at 350°C which is within the range of those obtained by the conventional technique of elaboration, proving that the material is not degraded using this novel route. It is mainly due to the good density and the absence of microcracks. Elaboration of legs with various geometry (cuboid and layered) was done to demonstrate the interest of this innovation manufacturing route. The benefit impact of the geometry was evaluated in term of voltages by a comparison measurement between a cuboid and a layered sample for which a remarkable gain of 16.5% (at an applied temperature of 74.7°C) was obtained for the layered sample due to a better thermal dissipation.

Flexible Ag2Se/Ag2S nanocomposite on carbon fabric optimized via interfaced engineered energy filtering effect for a textile based wearable thermoelectric generator

Wearable devices have become increasingly attractive in wearable electronics due to their advantages of environmental friendliness and foldability. The state-of-the-art thermoelectric system depends on inorganic semiconductors that show high electron mobility but lack mechanical stability and thermoelectric performance. Here, We have proposed a solvothermal method to grow Ag2Se/Ag2S nanocomposite on carbon fabric with outstanding properties, demonstrating excellent flexibility. The crystallographic analysis was performed for all samples through XRD and confirmed the orthorhombic Ag2Se and mono-clinic Ag2S. Further, the morphological analysis revealed the enhanced growth on the carbon fabric. We investigated the thermoelectric properties of Ag2Se/Ag2S nanocomposite and achieved a high power factor of 8.1 μW/mK2 which is twice as high as the percentage of the pure Ag2Se. Additionally, thermoelectric legs were fabricated using Ag2Se/Ag2S nanocomposite in a 2-pair module. They produced an output voltage of 0.1 mV to 7.4 mV at a temperature gradient (ΔT) of 3–8 K. This work is a promising approach for obtaining high-performance wearable thermoelectric device.

Brushy C-Decorated BiTe-Based Thermoelectric Film for Efficient Photodetection and Photoimaging.

Current strategies for simultaneously achieving high thermoelectric performance and high light absorption efficiency still suffer from complex steps and high costs. Herein, two kinds of amorphous thermoelectric films of n-type Bi2Te3 and p-type Bi0.5Sb1.5Te3 with high Seebeck coefficients were prepared by pulsed laser deposition (PLD) technology. In addition, C-decorated films with excellent light absorption efficiency at the junction of the thermoelectric legs were prepared by simple drop coating and reactive ion etching (RIE) method. The TE/C-RIE composite device exhibits excellent photodetection performance under the conditions of simulated natural light, monochromatic light, and high-frequency chopping. The maximum responsivity and specific detectivity of the device can reach 153.58 mV W-1 and 6.97 × 106 cm Hz1/2 W-1 (under simulated natural light), respectively. This represents an improvement rate of 85.91% compared to that of the pure TE device. Benefiting from the excellent photodetection efficiency of the device and integration advantage of PLD technology, the composite structure can be expanded into integrated photoimaging devices. The accurate identification of patterned light sources with letters (T, J, and U) and digitals (0-9) was successfully realized by associating the response electrical signals of each electrode with the position coordinates. This work provides valuable guidance for the design and fabrication of wide-spectrum photodetectors and complex optical imaging devices.

One‐Step‐Sintered GeTe‐Bi2Te3 Segmented Thermoelectric Legs with Robust Interface‐Connection Performance

AbstractSegmented thermoelectric (TE) legs are promising for improving heat‐electricity conversion efficiency, but their practical applications are still limited by the lack of cost‐effective interface‐connection technology. Here, an interface‐connection method for one‐step sintering of GeTe‐Bi2Te3 segmented TE legs is developed using mixtures of Al0.88Si0.12 and Ni (ASN) as diffusion barrier materials. Although the interface‐connection performance using Ni or Al0.88Si0.12 alone is poor, their mixtures can realize a compromise optimization of interface‐connection properties, simultaneously achieving a matched coefficient of thermal expansion, low contact resistivity, high shear strength, and high reliability. These robust interface‐connection properties can be attributed to the activation of the eutectic‐alloy Al0.88Si0.12 and the formation of appropriate reaction‐diffusion layers between ASN and GeTe/Bi2Te3 and between Al0.88Si0.12 and Ni in ASN. Finally, a remarkable energy conversion efficiency of ≈15.5% at a temperature difference of 449 K can be obtained in this segmented TE leg. Moreover, ASN can also be applied in fabricating n‐type PbTe‐Bi2Te3 segmented legs and multi‐pair TE devices, demonstrating the universality of this methodology. This work accelerates the development of robust, low‐cost, one‐step‐sintered segmented TE legs and promotes the use of eutectic alloys as “alloy glues” for advancing TE‐device connection technology.

Optimization Design and Performance Study of Wearable Thermoelectric Device Using Phase Change Material as Heat Sink.

Wearable thermoelectric generators have great potential to provide power for smart electronic wearable devices and miniature sensors by harnessing the temperature difference between the human body and the environment. However, the Thomson effect, the Joule effect, and heat conduction can cause a decrease in the temperature difference across the thermoelectric generator during operation. In this paper, phase change materials (PCMs) were employed as the heat sink for the thermoelectric generator, and the COMSOL software 6.1 was utilized to simulate and optimize the power generation processes within the heat sink. The results indicated that with a PCM height of 40 mm, phase transition temperature of 293 K, latent heat of 200 kJ/kg, phase transition temperature interval of 5 K, thermal conductivity of 50 W/(m·K), isobaric heat capacity of 2000 J/(Kg·K), density of 1000 kg/m3, and convective heat transfer coefficient of 10 W/(m·K), the device can maintain a temperature difference of 18-10 K for 1930 s when the thermoelectric leg height is 1.6 mm, and 3760 s when the thermoelectric leg height is 2.7 mm. These results demonstrate the correlation between the device's output performance and the dimensions and performance parameters of the PCM heat sink, thereby validating the feasibility of employing the PCM heat sink and the necessity for systematic investigations.

3D-printed Bi2Te3-based Thermoelectric Generators for Energy Harvesting and Temperature Response.

Thermoelectric generators (TEGs) are environmentally friendly energy harvesting technologies that hold great promise in the field of self-powered electronics and sensing. However, the current development of thermoelectric (TE) devices has largely lagged behind the development of thermoelectric materials, especially in the preparation of thermoelectric components with customizable shapes and excellent properties, which largely limits their practical applications. These issues can be effectively addressed by using 3D printing technology. Here, we print multiple p-type thermoelectric legs (pins) consecutively with this simple technique, and the printed TEGs have excellent thermal potential (288 μV K-1 at room temperature) and excellent temperature response properties, which exhibited an output voltage of 127.94 mV at a temperature difference (ΔT) of 40 K. The 3D-printed thermoelectric generator enables the collection of thermal energy. In addition, the device has excellent temperature sensing characteristics, and this temperature signal to electrical signal conversion is very rapid, which enables temperature sensing alarms in a wide temperature domain. Combining these features, an energy harvesting and electrical alarm concept for home-scale applications is proposed, which is expected to provide a diverse research idea for the application of next-generation thermoelectric devices.

Direct Melt-Calendaring of Highly Textured (Bi,Sb)2Te3 Thick Films: Superior Thermoelectric and Mechanical Performance via Strain Engineering.

The evolutions of chip thermal management and micro energy harvesting put forward urgent need for micro thermoelectric devices. Nevertheless, low-performance thermoelectric thick films as well as the complicated precision cutting process for hundred-micron thermoelectric legs still remain the bottleneck hindering the advancement of micro thermoelectric devices. In this work, an innovative direct melt-calendaring manufacturing technology is first proposed with specially designed and assembled equipment, that enables direct, rapid, and cost-effective continuous manufacturing of Bi2Te3-based films with thickness of hundred microns. Based on the strain engineering with external glass coating confinement and controlled calendaring deformation degree, enhanced thermoelectric performance has been achieved for (Bi,Sb)2Te3 thick films with highly textured nanocrystals, which can promote carrier mobility over 182.6 cm2 V-1 s-1 and bring out a record-high zT value of 0.96 and 1.16 for n-type and p-type (Bi,Sb)2Te3 thick films, respectively. The nanoscale interfaces also further improve the mechanical strength with excellent elastic modules (over 42.0GPa) and hardness (over 1.7GPa), even superior to the commercial zone-melting ingots and comparable to the hot-extrusion (Bi,Sb)2Te3 alloys. This new fabrication strategy is versatile to a wide range of inorganic thermoelectric thick films, which lays a solid foundation for the development of micro thermoelectric devices.

Performance analysis of four-stage thermoelectric cooler for focal plane infrared detectors

A cooler provides a low-temperature working environment for refrigerated infrared detection chips and is an indispensable component in infrared detectors that ensures their smooth operation. In this paper, a thermodynamic model of a heat-pipe-type four-stage thermoelectric cooler with a large temperature difference applied to a focal plane infrared detector is constructed. The heat leakage of the detector is calculated using the model. The performance indexes of the coordination performance coefficient and module utilization coefficient are used to unify the cooling capacity and economic performance of the device. The impression of the working current, heat pipe parameters, and cross-sectional area of the thermoelectric leg on the performance of cooler are analyzed. A Pareto optimal solution is obtained using an NSGA-II algorithm and TOPSIS decision. A low cooling temperature is obtained using a multistage thermoelectric cooler to achieve a large cooling temperature difference. When the working current is 5.65 A and the cross-sectional area is 4.5 mm2, the maximum cooling temperature difference reaches 110.6 °C, and the lowest cooling temperature reaches -83.6 °C. When the working temperature of the detector is -60 °C, the current and cross-sectional area corresponding to the optimal solution of cooling capacity-COP-power consumption are 1.51 A and 2.74 mm2, respectively.

Heat-Dissipation Design and 3D Printing of Ternary Silver Chalcogenide-Based Thermoelectric Legs for Enhancing Power Generation Performance.

Thermoelectric devices have received significant attention because of their potential for sustainable energy recovery. In these devices, a thermal design that optimizes heat transfer and dissipation is crucial for maximizing the power output. Heat dissipation generally requires external active or passive cooling devices, which often suffer from inevitable heat loss and heavy systems. Herein, the design of heat-sink integrated thermoelectric legs is proposed to enhance heat dissipation without external cooling devices, realized by finite element model simulation and 3D printing of ternary silver chalcogenide-based thermoelectric materials. Owing to the self-induced surface charges of the synthesized AgBiSe2 (n-type) and AgSbTe2 (p-type) particles, these particle-based colloidal inks exhibited high viscoelasticity, which enables the creation of complex heat-dissipation architectures via 3D printing. Power generators made from 3D-printed heat-dissipating legs exhibit higher temperature differences and output power than traditional cuboids, offering a new strategy for enhancing thermoelectric power generation.

A novel thermal management system for a cylindrical battery based on tubular thermoelectric generator

This study introduces an innovative thermal management system tailored for cylindrical Lithium-ion batteries. It integrates a tubular thermoelectric generator (TTEG) to handle both battery thermal management and the utilization of waste heat for power generation. The main focus lies in evaluating the waste heat recovery capabilities of the TTEG to enhance effective thermal management. The research investigates key geometric and operational parameters such as battery discharge rate (C-rate), thermocouple count (NTC), heat transfer coefficient (HTC), and thermoelectric leg height (HL) to comprehensively assess the overall system performance. The results highlight that integrating the TTEG improves thermal management and waste heat recovery in lithium-ion batteries. It demonstrates temperature reductions of up to 21 °C at a discharge rate of 3C compared to batteries without the TTEG thermal management system. Additionally, increasing the NTC leads to a rise in the maximum battery temperature, thereby enhancing waste heat recovery performance. For instance, increasing the number of thermocouples from 100 to 144 results in a substantial up to 70 % increase in TTEG voltage.Furthermore, enhancing HTC and HL positively impacts thermal performance, showing a significant decrease in the maximum battery temperature. Elevated HTC and HL also contribute to improving thermoelectric voltage, power, and conversion efficiency, highlighting their dual role in enhancing waste heat recovery. For instance, at peak conditions, there is a notable reduction of 2.66 °C in the maximum battery temperature with an HL of 12 mm compared to 4 mm. Additionally, increasing HTC from 10 to 20, particularly at maximum discharge, leads to a surge of 15.87 % in voltage and a substantial 34.28 % increase in output power.

A novel strategy of inserting radiation shields to enhance the performance of thermoelectric generator systems for industrial high-temperature heat recovery

Static thermoelectric generator (TEG) systems have been widely used for recovering the high-temperature heat from the industrial sector. To control the heat loss through the gap uncovered by the thermoelectric legs for system performance improvement, a novel strategy of inserting the radiation shields in the gap that introduced additional surface and spacing resistances and regulated the gap radiation loss, was proposed. With a constructed high-fidelity theoretical model which used the finite element method to consider the temperature-dependent properties of the thermoelectric materials, comprehensive comparisons were conducted between the systems with/without radiation shields and using three commonly adopted strategies to evaluate the effectiveness and potential of this strategy. Compared to the base case without radiation shields, inserting one radiation shield with an emissivity of 0.5 enhances the TEG efficiency and system power by 15 % and 9.5 % respectively. The system using the proposed strategy outperforms that using the commonly adopted strategies, especially the strategies of lowering the gap pressure and filling the gap with thermal insulation materials, highlighting the potential of the proposed strategy. Besides, the influences of the shield emissivity and number were studied; from it, less than two radiation shields made by the polished copper are recommended for practical applications.

General strategy for developing thick-film micro-thermoelectric coolers from material fabrication to device integration

Micro-thermoelectric coolers are emerging as a promising solution for high-density cooling applications in confined spaces. Unlike thin-film micro-thermoelectric coolers with high cooling flux at the expense of cooling temperature difference due to very short thermoelectric legs, thick-film micro-thermoelectric coolers can achieve better comprehensive cooling performance. However, they still face significant challenges in both material preparation and device integration. Herein, we propose a design strategy which combines Bi2Te3-based thick film prepared by powder direct molding with micro-thermoelectric cooler integrated via phase-change batch transfer. Accurate thickness control and relatively high thermoelectric performance can be achieved for the thick film, and the high-density-integrated thick-film micro-thermoelectric cooler exhibits excellent performance with maximum cooling temperature difference of 40.6 K and maximum cooling flux of 56.5 W·cm−2 at room temperature. The micro-thermoelectric cooler also shows high temperature control accuracy (0.01 K) and reliability (over 30000 cooling cycles). Moreover, the device demonstrates remarkable capacity in power generation with normalized power density up to 214.0 μW · cm−2 · K−2. This study provides a general and scalable route for developing high-performance thick-film micro-thermoelectric cooler, benefiting widespread applications in thermal management of microsystems.

Enhancing Bi2Te2.70Se0.30 Thermoelectric Module Performance through COMSOL Simulations

This research employs the COMSOL Multiphysics software (COMSOL 6.2) to conduct rigorous simulations and assess the performance of a thermoelectric module (TEM) meticulously crafted with alumina (Al2O3), copper (Cu), and Bi2Te2.70Se0.30 thermoelectric (TE) materials. The specific focus is on evaluating diverse aspects of the Bi2Te2.70Se0.30 thermoelectric generator (TEG). The TEM design incorporates Bi2Te2.70Se0.30 for TE legs of the p- and n-type positioned among the Cu layers, Cu as the electrical conductor, and Al2O3 serving as an electrical insulator between the top and bottom layers. A thorough investigation is conducted into critical parameters within the TEM, which include arc length, electric potential, normalized current density, temperature gradient, total heat source, and total net energy rate. The geometric configuration of the square-shaped Bi2Te2.70Se0.30 TEM, measuring 1 mm × 1 mm × 2.5 mm with a 0.25 mm Al2O3 thickness and a 0.125 mm Cu thickness, is scrutinized. This study delves into the transport phenomena of TE devices, exploring the impacts of the Seebeck coefficient (S), thermal conductivity (k), and electrical conductivity (σ) on the temperature differential across the leg geometry. Modeling studies underscore the substantial influence of S = ±2.41 × 10−3 V/K, revealing improved thermal conductivity and decreased electrical conductivity at lower temperatures. The findings highlight the Bi2Te2.70Se0.30 TEM’s high potential for TEG applications, offering valuable insights into design and performance considerations crucial for advancing TE technology.

Geometrical Optimization of Segmented Thermoelectric Generators (TEGs) Based on Neural Network and Multi-Objective Genetic Algorithm

In this study, a neural network and a multi-objective genetic algorithm were used to optimize the geometric parameters of segmented thermoelectric generators (TEGs) with trapezoidal legs, including the cold end width of thermoelectric (TE) legs (Wc), the ratios of cold-segmented length to the total lengths of the n- and p-legs (Sn,c and Sp,c), and the width ratios of the TE legs between the hot end and the cold end of the n- and p-legs (Kn and Kp). First, a neural network with high prediction accuracy was trained based on 5000 sets of parameters and the corresponding output power values of the TEGs obtained from finite element simulations. Then, based on the trained neural network, the multi-objective genetic algorithm was applied to optimize the geometric parameters of the segmented TEGs with the objectives of maximizing the output power (P) and minimizing the semiconductor volume (V). The optimal geometric parameters for different semiconductor volumes were obtained, and their variations were analyzed. The results indicated that the optimal Sn,c, Sp,c, Kn, and Kp remained almost unchanged when V increased from 52.8 to 216.2 mm3 for different semiconductor volumes. This work provides practical guidance for the design of segmented TEGs with trapezoidal legs.

Finite Element Analysis and Design of a Flexible Thermoelectric Generator with a Rhombus Gap Structure.

Flexible thermoelectric generators (f-TEGs) offer an opportunity to realize wearable, self-powered electronic devices. A typical f-TEG consists of flexible electrodes and rigid thermoelectric (TE) legs in a flexible package. In the realm of f-TEGs utilizing flexible electrodes and TE cuboids, our unwavering objective lies in the attainment of enhanced flexibility and elevated energy conversion efficiency. In this paper, we employ a quasi-three-dimensional thermal model to design an f-TEG with a rhombus gap structure (E/A-RhTEG) with its optimized performance validated by simulation and experiment. Additionally, the lateral and vertical thermal resistances are introduced to further explain the optimizing principle in the f-TEG's output performance. Compared with the conventional TEG with a rectangular air gap structure (E/A-ReTEG), E/A-RhTEG demonstrates improved energy conversion efficiency to some extent. Simulation results indicate that the output power and energy conversion efficiency of a 25-np-pair E/A-RhTEG at a 30 K temperature gradient reach 8.45 mW and 2.55%, which represent a performance improvement of 3.09 and 6.28%, respectively, compared to E/A-ReTEG. To further elucidate the optimization principle in the performance of f-TEGs, additional considerations are given to the lateral and vertical resistances. In this study, E/A-RhTEG comprising 25 np pairs is fabricated utilizing TE cuboids. Experimental findings indicate that E/A-RhTEG exhibits a voltage output of 127.07 mV when subjected to a temperature difference of 30 K, which demonstrates a performance enhancement of 4.06% compared to E/A-ReTEG. Furthermore, this study also demonstrates its implementation when wrapped around a curved surface and successfully achieves a self-powered device system after device performance optimization.

Multiscale functionalized graphene origami metamaterials enable programming thermoelectric performance of flexible energy harvesters

Origami engineering stands out as one of the prominent approaches for fine tuning the multiphysical properties of energy materials. Employing first-principle calculations at the nanoscale, we explore the mechano-thermoelectric properties of graphene origami metamaterials functionalized by hydrogen (H), nitrogen (N), oxygen (O), and fluorine (F) adatoms. Our computational results reveal that functionalizing carbon (C) atoms induce buckling in the pristine graphene, transitioning carbon atoms from sp2 (for pristine graphene sheet) to hybridized sp3 orbital to fold the graphene origami. The functionalized graphene origami metamaterials, adopting the Miura-ori architecture, exhibit anisotropic mechanical properties and an unprecedented negative Poisson's ratio (NPR) of up to −0.8. Non-symmetrical functionalization breaks the inherent symmetry of graphene, resulting in a robust non-zero electronic band gap. This characteristic makes the graphene origami metamaterial a compelling contender for thermoelectric applications, since they offer an electronic figure of merit that exceed 200 at room temperature (Graphene-H), surpassing that of the majority of 2D thermoelectric materials can offer. Resorting to the finite element approach, we explore the origami-based thermoelectric legs in nanogenerators at mesoscale. The folding capability of origami architectures offer tunable heat insulation in order to realize next generation of thermoelectric legs. Compared to conventional cuboid leg thermoelectric nanogenerators, thermoelectric conversion efficiency of origami metamaterials can be two orders of magnitude higher; an enhancement that is significantly governed by their folding angle. The underlying principles governing the multiphysics performance of multiscale origami-based thermoelectric materials impart novel design concepts for customizing the thermoelectric performance of shape-changing low-dimensional metamaterials and energy-related devices.