Organic thermoelectric(OTE)materials have been considered to be promising candidates for large area and low‐cost wearable devices owing to their tailorable molecular structure,intrinsic flexibility,and prominent solu...Organic thermoelectric(OTE)materials have been considered to be promising candidates for large area and low‐cost wearable devices owing to their tailorable molecular structure,intrinsic flexibility,and prominent solution processability.More importantly,OTE materials offer direct energy conversion from the human body,solid‐state cooling at low electric consumption,and diversified functions.Herein,we summarize recent developments of OTE materials and devices for smart applications.We first review the fundamentals of OTE materials from the viewpoint of thermoelectric performance,mechanical properties and bionic functions.Second,we describe OTE devices in flexible generators,photothermoelectric detectors,self‐powered sensors,and ultra‐thin cooling elements.Finally,we present the challenges and perspectives on OTE materials as well as devices in wearable electronics and fascinating applications in the Internet of Things.展开更多
In this work,Ag/Ag_(2)Se composite films with excellent thermoelectric(TE)properties and flexibility are prepared based on a simple one-pot method.By adjusting the nominal ratios of Ag/Se,an optimal Ag/Ag_(2)Se compos...In this work,Ag/Ag_(2)Se composite films with excellent thermoelectric(TE)properties and flexibility are prepared based on a simple one-pot method.By adjusting the nominal ratios of Ag/Se,an optimal Ag/Ag_(2)Se composite film shows a large power factor of~2275 μW m^(-1) K^(-2) at 300 K.Such an outstand-ing TE performance of the composite film is due to the unique microstructure and the synergistic effect between the Ag and Ag_(2)Se.Meanwhile,the composite film also shows outstanding flexibility(~91.8%of the initial electrical conductivity is maintained,and the S is unchanged after 1500 bending cycles with a bending radius of 4 mm).Furthermore,a 4-leg flexible TE generator assembled with the optimal film produces a voltage of 14.06 mV and 4.96 μW at a temperature difference of 30.4 K.This work provides a new inspiration for the preparation of flexible Ag_(2)Se-based films with excellent TE performance near room temperature.展开更多
Bi_(2)Se_(3)-based flexible thin film with high thermoelectric performance is promising for the waste heat recovery technology.In this work,a novel post-selenization method is employed to prepare n-type Bi_(2)Se_(3)fl...Bi_(2)Se_(3)-based flexible thin film with high thermoelectric performance is promising for the waste heat recovery technology.In this work,a novel post-selenization method is employed to prepare n-type Bi_(2)Se_(3)flexible thin films with highly textured structure.The strengthened texture and Se vacancy optimization can be simultaneously achieved by optimizing the selenization temperature.The highly oriented texture leads to the increased carrier mobility and results in a high electric conductivity of~290.47 S·cm^(-1)at 623 K.Correspondingly,a high Seebeck coefficient(>110μW·K-1)is obtained due to the reduced carrier concentration,induced by optimizing vacancy engineering.Consequently,a high power factor of 3.49μW·cm^(-1)·K^(-2)at 623 K has been achieved in asprepared highly-bendable Bi_(2)Se_(3)flexible thin films selenized at 783 K.This study introduces an effective post-selenization method to tune the texture structure and vacancies of Bi_(2)Se_(3)flexible thin films,and correspondingly achieves high thermoelectric performance.展开更多
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 ac...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.展开更多
An automated thin-layer flow cell electrodeposition system was developed for growing Bi2Te3 thin film by ECALE. The dependence of the Bi and Te deposition potentials on Pt electrode was studied. In the first attempt, ...An automated thin-layer flow cell electrodeposition system was developed for growing Bi2Te3 thin film by ECALE. The dependence of the Bi and Te deposition potentials on Pt electrode was studied. In the first attempt, this reductive Te underpotential deposition （UPD）/reductive Bi UPD cycle was performed to 100 layers. A better linearity of the stripping charge with the number of cycles has been shown and confirmed a layer-by-layer growth mode, which is consistent with an epitaxial growth. The 4∶3 stoichiometric ratio of Bi to Te suggests that the incomplete charge transfer in HTeO+2 reduction excludes the possibility of Bi2Te3 formation. X-ray photoelectron spectroscopy （XPS） analysis also reveals that the incomplete charge transfer in HTeO+2 occurs in Te direct deposition. The effective way of depositing Bi2Te3 on Pt consists in oxidative Te UPD and reductive Bi UPD. The thin film deposited by this procedure was characterized by X-ray diffraction（XRD）, scanning electron microscopy（SEM） and X-ray photoelectron spectroscopy（XPS）. A polycrystalline characteristic was confirmed by XRD. The 2∶3 stoichiometric ratio was confirmed by XPS. The SEM image indicates that the deposit looks like a series of buttons about （0.30.4 μm） in diameter, which is corresponding with calculated thickness of the epitaxial film. This suggests that the particle growth appears to be linear with the number of cycles, as it is consistent with a layer by layer growth mode.展开更多
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 f...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.展开更多
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 int...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.展开更多
Thermoelectric thin film has attracted a lot of attention due to its potential in fabricating micropower generator in chip sensors for internet of things(IoT).However,the undeveloped performance of n-type thermoelectr...Thermoelectric thin film has attracted a lot of attention due to its potential in fabricating micropower generator in chip sensors for internet of things(IoT).However,the undeveloped performance of n-type thermoelectric thin film limits its widely application.In this work,a facile post-selenization diffusion reaction method is employed to introduce Se into Bi_(2)Te_(3)thin films,in order to optimize the carrier transport properties.Experimental and theoretical calculation results indicate that the carrier concentration decreases and density of states increases after Se doping,leading to the enhancement of Seebeck coefficient.Further,adjusting the diffusion reaction temperature can maintain the carrier concentration while increasing the mobility simultaneously,resulting in a high power factor of 1.5 mW/(m·K^(2)),which is eight times higher than that of the pristine Bi_(2)Te_(3)thin films.Subsequently,a thin film device fabricated by the present Se-doped Bi_(2)Te_(3)thin films shows the highest output power of 60.20 nW under the temperature difference of 37 K,indicating its potential for practical use.展开更多
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 s...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.展开更多
基金supported by the National Key Research and Development Program of China(2017YFA0204700 and 2018YFE0200700)the National Natural Science Foundation of China(21805285,22021002,21905276,61971396)+2 种基金the Natural Science Foundation of Beijing(4202077)Beijing National Laboratory for Molecular Sciences(BNLMS201912)UCAS(Y954011XX2)and CAS(ZDBS‐LY‐SLH034).
文摘Organic thermoelectric(OTE)materials have been considered to be promising candidates for large area and low‐cost wearable devices owing to their tailorable molecular structure,intrinsic flexibility,and prominent solution processability.More importantly,OTE materials offer direct energy conversion from the human body,solid‐state cooling at low electric consumption,and diversified functions.Herein,we summarize recent developments of OTE materials and devices for smart applications.We first review the fundamentals of OTE materials from the viewpoint of thermoelectric performance,mechanical properties and bionic functions.Second,we describe OTE devices in flexible generators,photothermoelectric detectors,self‐powered sensors,and ultra‐thin cooling elements.Finally,we present the challenges and perspectives on OTE materials as well as devices in wearable electronics and fascinating applications in the Internet of Things.
基金National Natural Science Foundation of China (Nos. 92163118 and 51972234).
文摘In this work,Ag/Ag_(2)Se composite films with excellent thermoelectric(TE)properties and flexibility are prepared based on a simple one-pot method.By adjusting the nominal ratios of Ag/Se,an optimal Ag/Ag_(2)Se composite film shows a large power factor of~2275 μW m^(-1) K^(-2) at 300 K.Such an outstand-ing TE performance of the composite film is due to the unique microstructure and the synergistic effect between the Ag and Ag_(2)Se.Meanwhile,the composite film also shows outstanding flexibility(~91.8%of the initial electrical conductivity is maintained,and the S is unchanged after 1500 bending cycles with a bending radius of 4 mm).Furthermore,a 4-leg flexible TE generator assembled with the optimal film produces a voltage of 14.06 mV and 4.96 μW at a temperature difference of 30.4 K.This work provides a new inspiration for the preparation of flexible Ag_(2)Se-based films with excellent TE performance near room temperature.
基金financially supported by the Natural Science Foundations of Shandong Province(No.ZR2023ME001)the China Postdoctoral Science Foundation(No.2023M732609)+1 种基金ShangRao City of Jiangxi Province(China)(No.2022A006)Doctoral Research Initiation Fund of Weifang University(No.2023BS01)。
文摘Bi_(2)Se_(3)-based flexible thin film with high thermoelectric performance is promising for the waste heat recovery technology.In this work,a novel post-selenization method is employed to prepare n-type Bi_(2)Se_(3)flexible thin films with highly textured structure.The strengthened texture and Se vacancy optimization can be simultaneously achieved by optimizing the selenization temperature.The highly oriented texture leads to the increased carrier mobility and results in a high electric conductivity of~290.47 S·cm^(-1)at 623 K.Correspondingly,a high Seebeck coefficient(>110μW·K-1)is obtained due to the reduced carrier concentration,induced by optimizing vacancy engineering.Consequently,a high power factor of 3.49μW·cm^(-1)·K^(-2)at 623 K has been achieved in asprepared highly-bendable Bi_(2)Se_(3)flexible thin films selenized at 783 K.This study introduces an effective post-selenization method to tune the texture structure and vacancies of Bi_(2)Se_(3)flexible thin films,and correspondingly achieves high thermoelectric performance.
基金supported by the National Key R&D Program of China(Grant No.2018YFA0702100)the Zhejiang Provincial Key R&D Program of China(Grant No.2021C05002)+1 种基金the Beijing Nova Programme Interdisciplinary Cooperation Project(Grant Nos.Z191100001119019 and Z191100001119013)the Fundamental Research Funds for the Central Universities。
文摘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.
基金Project(50401008) supported by the Chinese National Natural Science Foundation Project(2004CCA03200) supportedby the National Basic Research Program
文摘An automated thin-layer flow cell electrodeposition system was developed for growing Bi2Te3 thin film by ECALE. The dependence of the Bi and Te deposition potentials on Pt electrode was studied. In the first attempt, this reductive Te underpotential deposition （UPD）/reductive Bi UPD cycle was performed to 100 layers. A better linearity of the stripping charge with the number of cycles has been shown and confirmed a layer-by-layer growth mode, which is consistent with an epitaxial growth. The 4∶3 stoichiometric ratio of Bi to Te suggests that the incomplete charge transfer in HTeO+2 reduction excludes the possibility of Bi2Te3 formation. X-ray photoelectron spectroscopy （XPS） analysis also reveals that the incomplete charge transfer in HTeO+2 occurs in Te direct deposition. The effective way of depositing Bi2Te3 on Pt consists in oxidative Te UPD and reductive Bi UPD. The thin film deposited by this procedure was characterized by X-ray diffraction（XRD）, scanning electron microscopy（SEM） and X-ray photoelectron spectroscopy（XPS）. A polycrystalline characteristic was confirmed by XRD. The 2∶3 stoichiometric ratio was confirmed by XPS. The SEM image indicates that the deposit looks like a series of buttons about （0.30.4 μm） in diameter, which is corresponding with calculated thickness of the epitaxial film. This suggests that the particle growth appears to be linear with the number of cycles, as it is consistent with a layer by layer growth mode.
基金supported by the National Key Research and Development Program of China(2020YFA0715000)the Guangdong Basic and Applied Basic Research Foundation(2020A1515110250,2021B1515120041)+1 种基金the Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory(XHT2020-005)the Fundamental Research Funds for the Central Universities(2020IVA068,2021lll007JC)
文摘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.
基金supported by the National Natural Science Foundation of China(52272235)supported by the Fundamental Research Funds for the Central Universities(WUT:2021III016GX).
文摘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.
基金the Technology Plan Project of Shenzhen(20220810154601001 and JCYJ20220531103601003)National Natural Science Foundation of China(No.62274112)Guangdong Basic and Applied Basic Research Foundation(2019A1515110107 and 2022A1515010929)。
文摘Thermoelectric thin film has attracted a lot of attention due to its potential in fabricating micropower generator in chip sensors for internet of things(IoT).However,the undeveloped performance of n-type thermoelectric thin film limits its widely application.In this work,a facile post-selenization diffusion reaction method is employed to introduce Se into Bi_(2)Te_(3)thin films,in order to optimize the carrier transport properties.Experimental and theoretical calculation results indicate that the carrier concentration decreases and density of states increases after Se doping,leading to the enhancement of Seebeck coefficient.Further,adjusting the diffusion reaction temperature can maintain the carrier concentration while increasing the mobility simultaneously,resulting in a high power factor of 1.5 mW/(m·K^(2)),which is eight times higher than that of the pristine Bi_(2)Te_(3)thin films.Subsequently,a thin film device fabricated by the present Se-doped Bi_(2)Te_(3)thin films shows the highest output power of 60.20 nW under the temperature difference of 37 K,indicating its potential for practical use.
基金Project supported by the National Natural Science Foundation of China(Nos.11972363 and12272401)the Opening Project of State Key Laboratory of Solid Lubrication(Lanzhou Institute of Chemical Physics)(No.LSL-20012001)the Research Fund of State Key Laboratory of Mechanics and Control of Mechanical Structures(Nanjing University of Aeronautics and Astronautics)(No.MCMS-E-0221G01)。
文摘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.
