Interfacial behavior of a thermoelectric film bonded to a graded substrate

To improve the thermoelectric converting performance in applications such as power generation,reutilization of heat energy,refrigeration,and ultrasensitive sensors in scramjet engines,a thermoelectric film/substrate system is widely designed and applied,whose interfacial behavior dominates the strength and service life of thermoelectric devices.Herein,a theoretical model of a thermoelectric film bonded to a graded substrate is proposed.The interfacial shear stress,the normal stress in the thermoelectric film,and the stress intensity factors affected by various material and geometric parameters are comprehensively studied.It is found that adjusting the inhomogeneity parameter of the graded substrate,thermal conductivity,and current density of the thermoelectric film can reduce the risk of interfacial failure of the thermoelectric film/graded substrate system.Selecting a stiffer and thicker thermoelectric film is advantageous to the reliability of the thermoelectric film/graded substrate system.The results should be of great guiding significance for the present and upcoming applications of thermoelectric materials in various fields.

An overview of thermoelectric films:Fabrication techniques,classification,and regulation methods

Thermoelectric materials have aroused widespread concern due to their unique ability to directly convert heat to electricity without any moving parts or noxious emissions.Taking advantages of two-dimensional structures of thermoelectric films,the potential applications of thermoelectric materials are diversified,particularly in microdevices.Well-controlled nanostructures in thermoelectric films are effective to optimize the electrical and thermal transport,which can significantly improve the performance of thermoelectric materials.In this paper,various physical and chemical approaches to fabricate thermoelectric films,including inorganic,organic,and inorganic–organic composites,are summarized,where more attentions are paid on the inorganic thermoelectric films for their excellent thermoelectric responses.Additionally,strategies for enhancing the performance of thermoelectric films are also discussed.

Preparation of Bi_(2-x)Sb_xTe_3 thermoelectric films by electrodeposition

Bi2-xSbxTe3 thermoelectric films were electrochemically deposited from the solution containing Bi^3＋, HTeO2^＋and SbO^＋. ESEM （environmental scanning electron microscope） investigations indicated that the crystalline state of Bi2-xSbxTe3 films transformed from equiaxed crystal to dendritic crystal with the negative shift of deposition potential. XRD and EDS were used to characterize the structure and composition of the electrodeposited films. The Seebeck coefficient and the temperature dependence of the resistance of Bi2-xSbxTe3 films were measured. The results showed that the composition of the film electrodeposited at -0.5 V is Bi2-xSbxTe3 with the largest Seebeck coefficient of 213 μV·K^-1.

Ultrafast Laser-Induced Excellent Thermoelectric Performance of PEDOT:PSS Films

Because poly(3,4-ethylenedioxythiophene)-poly(styrenesulfonate)(PEDOT:PSS)is water processable,thermally stable,and highly conductive,PEDOT:PSS and its composites have been considered to be one of the most promising flexible thermoelectric materials.However,the PEDOT:PSS film prepared from its commercial aqueous dispersion usually has very low conductivity,thus cannot be directly utilized for TE applications.Here,a simple environmental friendly strategy via femtosecond laser irradiation without any chemical dopants and treatments was demonstrated.Under optimal conditions,the electrical conductivity of the treated film is increased to 803.1 S cm^(-1)from 1.2 S cm^(-1)around three order of magnitude higher,and the power factor is improved to 19.0μW m^(-1)K^(-2),which is enhanced more than 200 times.The mechanism for such remarkable enhancement was attributed to the transition of the PEDOT chains from a coil to a linear or expanded coil conformation,reduction of the interplanar stacking distance,and the removal of insulating PSS with increasing the oxidation level of PEDOT,facilitating the charge transportation.This work presents an effective route for fabricating high-performance flexible conductive polymer films and wearable thermoelectric devices.

On-Chip Micro Temperature Controllers Based on Freestanding Thermoelectric Nano Films for Low-Power Electronics

Multidimensional integration and multifunctional com-ponent assembly have been greatly explored in recent years to extend Moore’s Law of modern microelectronics.However,this inevitably exac-erbates the inhomogeneity of temperature distribution in microsystems,making precise temperature control for electronic components extremely challenging.Herein,we report an on-chip micro temperature controller including a pair of thermoelectric legs with a total area of 50×50μm^(2),which are fabricated from dense and flat freestanding Bi2Te3-based ther-moelectric nano films deposited on a newly developed nano graphene oxide membrane substrate.Its tunable equivalent thermal resistance is controlled by electrical currents to achieve energy-efficient temperature control for low-power electronics.A large cooling temperature difference of 44.5 K at 380 K is achieved with a power consumption of only 445μW,resulting in an ultrahigh temperature control capability over 100 K mW^(-1).Moreover,an ultra-fast cooling rate exceeding 2000 K s^(-1) and excellent reliability of up to 1 million cycles are observed.Our proposed on-chip temperature controller is expected to enable further miniaturization and multifunctional integration on a single chip for microelectronics.

High-sensitivity self-powered temperature/pressure sensor based on flexible Bi-Te thermoelectric film and porous microconed elastomer

Electronic skins are artificial skin-type multifunctional sensors,which hold great potentials in intelligent robotics,limb prostheses and human health monitoring.However,it is a great challenge to independently and accurately read various physical signals without power supplies.Here,a self-powered flexible temperature-pressure bimodal sensor based on high-performance thermoelectric films and porous microconed conductive elastic materials is presented.Through introducing flexible heat-sink design and harvesting body heat energy,the thin-film thermoelectric device could not only precisely sense temperature signal but also drive the pressure sensor for detecting external tactile stimulus.The integration of Bi-Te based thermoelectric film with high stability in wide temperature range enables the sensor to sense the ambient temperature with high resolution(<0.1 K)as well as excellent sensitivity(3.77 mV K^(-1)).Meanwhile,the porous microconed elastomer responds to pressure variation with low-pressure detection(16 Pa)and a high sensitivity of 37 kPa^(-1).Furthermore,the bimodal sensor could accurately and simultaneously monitor human wrist pulse and body temperature in real time,which demonstrates promising applications in self-powered electronic skins for human health monitoring systems.

Electrodeposition and characterization of thermoelectric Bi_2Se_3 thin films

Bi2Se3 thin films were electrochemically deposited on Ti and indium tin oxide-coated glass substrates, respectively, at room temperature, using Bi（NO3）3·5H2O and SeO2 as starting materials in diluted HNO3 solution. A conventional three-electrode cell was used with a platinum sheet as a counter electrode, and a saturated calomel electrode was used as a reference electrode. The films were annealed in argon atmosphere. The influence of cold isostatic pressing before annealing on the microstructure and thermoelectric properties of the films was investigated. X-ray diffraction analysis indicates that the film grown on the indium tin oxide-coated glass substrate is pure rhombohedral Bi2Se3, and the film grown on the Ti substrate consists of both rhombohedral and orthorhombic Bi2Se3.

Effects of Thickness and Temperature on Thermoelectric Properties of Bi2Te3-Based Thin Films

Bi_2Te_3 thin films and GeTe/B_2Te_3 superlattices of different thicknesses are prepared on the silicon dioxide substrates by magnetron sputtering technique and thermally annealed at 573 K for 30 min. Thermoelectric（TE）measurements indicate that optimal thickness and thickness ratio improve the TE performance of Bi_2Te_3 thin films and GeTe/B_2Te_3 superlattices, respectively. High TE performances with figure-of-merit（ZT） values as high as 1.32 and 1.56 are achieved at 443 K for 30 nm and 50 nm Bi_2Te_3 thin films, respectively. These ZT values are higher than those of p-type Bi_2Te_3 alloys as reported. Relatively high ZT of the GeTe/B_2Te_3 superlattices at 300-380 K were 0.62-0.76. The achieved high ZT value may be attributed to the unique nano-and microstructures of the films,which increase phonon scattering and reduce thermal conductivity. The results indicate that Bi_2Te_3-based thin films can serve as high-performance materials for applications in TE devices.

Enhanced Electrical Properties of Bi_(2−x)Sb_(x)Te_(3) Nanoflake Thin Films Through Interface Engineering

The structure–property relationship at interfaces is difficult to probe for thermoelectric materials with a complex interfacial microstructure.Designing thermoelectric materials with a simple,structurally-uniform interface provides a facile way to understand how these interfaces influence the transport properties.Here,we synthesized Bi_(2−x)Sb_(x)Te_(3)(x=0,0.1,0.2,0.4)nanoflakes using a hydrothermal method,and prepared Bi_(2−x)Sb_(x)Te_(3) thin films with predominantly(0001)interfaces by stacking the nanoflakes through spin coating.The influence of the annealing temperature and Sb content on the(0001)interface structure was systematically investigated at atomic scale using aberration-corrected scanning transmission electron microscopy.Annealing and Sb doping facilitate atom diffusion and migration between adjacent nanoflakes along the(0001)interface.As such it enhances interfacial connectivity and improves the electrical transport properties.Interfac reactions create new interfaces that increase the scattering and the Seebeck coefficient.Due to the simultaneous optimization of electrical conductivity and Seebeck coefficient,the maximum power factor of the Bi_(1.8)Sb_(0.2)Te_(3) nanoflake films reaches 1.72 mW m^(−1)K^(−2),which is 43%higher than that of a pure Bi_(2)Te_(3) thin film.

High-Performance Sb-Doped GeTe Thermoelectric Thin Film and Device

GeTe-based materials have attracted significant attention as high-efficiency thermoelectric materials for mid-temperature applications.However,GeTe thin-film materials with thermoelectric performances comparable to that of their bulk counterparts have not yet been reported,because of their unsatisfactory electrical and thermal properties caused by their poor crystal quality and high carrier concentration.Herein,a series of Sb-doped GeTe films and devices with remarkable thermoelectric performances are presented.These films are prepared through magnetron sputtering deposition at 553 K and exhibit a unique microstructure that consists of coarse-and fine-sized grains with high crystallization quality.The fine grains enhance the scattering associated with phonon transport and the coarse grains provide electron transport channels,which can suppress the thermal conductivity without obviously sacrificing the electrical conductivity.Moreover,Sb doping can effectively optimize the carrier concentration and increase the carrier effective mass,while introducing point defects and stacking faults to further scatter the phonon transport and decrease the thermal conductivity.Consequently,a peak power factor of 22.37μW cm−1 K−2 is obtained at 703 K and a maximum thermoelectric figure of merit of 1.53 is achieved at 673 K,which are substantially larger than the values reported in the existing literature.A flexible thermoelectric generator is designed and fabricated using Sb-doped GeTe films deposited on polyimide and achieves a maximum output power density of 2.22×103 W m−2 for a temperature difference of 300 K.