TE Materials Research Articles

Exploring the thermoelectric performance of NiFeMnAl and ZnFeVAl as novel quaternary Heusler compounds

Quaternary Heusler (QH) compounds, characterized by the chemical formula XX’YZ, are highly regarded in the energy materials sector due to their versatile electronic structures. The current study focuses on synthesizing novel QH compounds, NiFeMnAl and ZnFeVAl, through arc-melting followed by hot-pressing at 1073 K. Maximum Seebeck coefficients were exhibited ∼ −20.48 μV/K and ∼ −17.25 μV/K at 773 K for ZnFeVAl and NiFeMnAl, respectively. The evaluated power factor was ∼ 0.058 mWm−1K−2 for NiFeMnAl and ∼ 0.020 mWm−1K−2 for ZnFeVAl at 773 K. Furthermore, the lattice thermal conductivity (κl) was exhibited ∼ 8.73 Wm−1K−1 for NiFeMnAl and ∼ 6.92 Wm−1K−1 for ZnFeVAl at 773 K, with ZnFeVAl exhibiting a ∼ 20.73 % lower κl attributed to chemical bonding distortion arising from differences in constituent element electronegativity. Hence, these novel compounds offer a promising avenue for further research in TE materials, aiming to realize higher-performance materials for practical TE device applications.

Synergistic Suppression of Bipolar Effect and Lattice Thermal Conductivity Leading to High Average Figure of Merit in Bi0.4Sb1.6Te3 Materials through Alloying with AgSbTe2.

Bismuth telluride-based materials have been widely used in commercial thermoelectric applications due to their excellent thermoelectric performance in the near-room-temperature range, yet further improvement of their thermoelectric properties is still necessary. Moreover, the narrow band gap of these materials results in a bipolar effect at elevated temperatures, which causes severe degradation of the thermoelectric performance. In this work, the commercial Bi0.4Sb1.6Te3 was alloyed with AgSbTe2 by using high-energy ball milling method combined with spark plasma sintering. It was found that ball milling can effectively reduce the lattice thermal conductivity of the samples. The alloying of AgSbTe2 leads to a gradual increase in hole carrier concentration, resulting in an enhanced electrical conductivity and optimized power factor. Additionally, the bipolar effect is also weakened due to the increased hole carrier concentration. Furthermore, the substitution of Ag in the Bi/Sb sublattice causes further reduction in the lattice thermal conductivity. Ultimately, the sample alloyed with 0.15 wt % AgSbTe2 demonstrates its best thermoelectric performance with a maximum zT of 1.35 at 393 K, showing a 20.5% improvement compared to the commercial sample. Besides, its average zT reaches a high value of 1.25 between 303 and 483 K, with a 27.6% improvement compared to that of the commercial sample.

A Polymer Film with Very High Seebeck Coefficient and Overall Thermoelectric Properties by Secondary Doping, Dedoping Engineering and Ionic Energy Filtering

AbstractThermoelectric (TE) materials are significant for sustainable development because they can be used to harvest waste heat into electricity. Organic TE materials have unique merits including high mechanical flexibility, low cost, and low intrinsic thermal conductivity. But their TE properties particularly the Seebeck coefficient are notably lower than the inorganic counterparts. Here, a poly(3,4‐ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS) film is reported with a very high Seebeck coefficient and figure of merit (zT) at room temperature through secondary doping, dedoping engineering, and ionic energy filtering. The PEDOT:PSS films are successively treated with acid, base, and vitamin C that is a reductant, and then coated with 1‐ethyl‐3‐methylimidazolium dicyanamide (EMIM:DCA) that is an ionic liquid. This can exhibit a record‐high Seebeck coefficient and power factor of 111 µV K−1 and 1285 µW m−1 K−2, respectively, and the corresponding zT value is 1.05. This is the highest zT value for polymers and polymer composites, and it is comparable to that of the best inorganic TE materials.

PEDOT:PSS Films With Very High Thermoelectric Properties Through Water‐Swollen Assisted Reduction With a Tetrakis(dimethylamino)ethylene Solution

AbstractThermoelectric (TE) materials have attracted significant attention because they can be used to directly harvest waste heat into electricity. Organic TE materials like poly(3,4‐ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) have advantages including high mechanical flexibility, low cost, and low intrinsic thermal conductivity. However, their TE properties are notably inferior to their inorganic counterparts. Here, PEDOT:PSS films with very high thermoelectric properties through the sequential treatments with H2SO4, water, and ethanol solution of tetrakis(dimethylamino)ethylene (TDAE) are reported for the first time. The PEDOT:PSS films can exhibit a Seebeck coefficient of 58.2 µV K−1 and electrical conductivity of 1552 S cm−1, and the corresponding power factor is 526 µW m−1 K−2. The water treatment prior to the TDAE solution treatment is crucial for the high TE properties of PEDOT:PSS films. Without the water treatment, the control PEDOT:PSS films exhibit a Seebeck coefficient of only 32.4 µV K−1 and electrical conductivity of 1124 S cm−1, and the corresponding power factor is only 118 µW m−1 K−2. The effect of the water treatment on the Seebeck coefficient is attributed to the swelling of PEDOT:PSS films, which facilitates the penetration of TDAE from solution into the polymer films and thus the reduction of PEDOT:PSS.

Flexible polyester-embedded thermoelectric device with Bi2Te3 and Te legs for wearable power generation

This study presents an approach for powering wearable sensors by integrating nanostructured bismuth telluride (Bi2Te3 and Te legs) into flexible polyester substrates. The choice of polyester as the substrate is because it is widely used in clothing, especially in items such as shirts, blouses, dresses, and sportswear. This enables seamless integration with wearable devices. By capturing wasted body heat, our small and flexible thermoelectric generators (TEGs) offer long-term operation without the need to plug the batteries. We demonstrate the feasibility of using commercially available polyester for reproducible electrochemical deposition of highly oriented Bi2Te3 and Te material. Through electrodeposition, we embed Bi2Te3 and Te legs within the flexible polyester, creating a cost-effective and easily scalable hybrid system for wearable energy harvesting.Our optimized TEG design, which can be worn on the arm or forehead, achieves impressive power density compared to existing state-of-the-art solutions. With a mere 3.5 °C temperature difference, only two pairs of p- and n-type legs, and a thickness of approximately 15 µm, our TEG generates a maximum open circuit voltage of ∼0.1 mV and a maximum power density of ∼0.04 mW·K-1·cm−2. With 250 pairs, 10 mV can be reached. This cost-effective design also integrates electrical contacts, surpassing previous flexible TEG performances. These advancements make our TEGs suitable for driving microwatt-level electronic sensors and open new avenues for efficient energy harvesting in wearable applications.

Exploring novel Na4XS (X = Se, Te) materials for UV protection and photovoltaic efficiency: First-principles approach

Novel chalcogenide materials exhibit remarkable thermal stability along with regulating optoelectronic properties. The structural, optoelectronic, and transport properties of Na4XS (X = Se, Te) materials were investigated using the most advanced density function theory. The calculated cohesive and formation energies confirm the stable nature of the studied materials. The study of their band structure profile reveals that their materials have a direct band gap and exhibit characteristics of a semiconducting nature. The determined peaks in the materials’ computed reflectance spectra suggest that they have the potential to be UV-reflective materials. This could lead to their potential use in UV-shielding devices. The negative Seebeck coefficients of the studied materials specify that they possess an n-type conductivity nature. Based on their direct energy gap, stable structure, adjustable optoelectronic performance, and remarkable thermal nature, they have significant potential for a wide range of novel and advanced technological applications.

Atomistic oxidation mechanism of Bi0.5Sb1.5Te3 (0001) surface

Surface oxidation can potentially influence transport properties of thermoelectric materials and service performance of thermoelectric devices. Here, the oxidation mechanism of the (0001) surface of a widely used p-type TE material, Bi0.5Sb1.5Te3 (BST), was investigated using spherical aberration corrected scanning transmission electron microscopy (STEM). Combining atomic resolution STEM and density function theory (DFT), it was revealed that oxidation occurs at room temperature in the dry air through O diffusion into the surface quintuple layer, facilitating formation of both cation and anion vacancies, weakening the Bi-Te and Sb-Te bonds, leading to oxidation product Sb2O3, amorphous Te, and Bi-rich Bi2Te3. Formation of a thin O-rich cation-deficient quintuple layer on the surface and the Bi-rich BST region can significantly reduce the interfacial reaction between BST and Ni electrode, as the reaction layer thickness is reduced by 75% after the surface oxidation. This work provides essential structural information on surface oxidation mechanism and its influence on properties and performance of TE materials and devices.

Experimental study on energy storage characteristics of packed bed using different solid materials

The packed bed energy storage system can solve the mismatch between solar energy supply and demand at a low cost. The physical properties of storage materials have a decisive impact on the performance of storage systems. Different scenarios may require different storage materials. Studying the impact of storage materials on storage characteristics is crucial. However, the comparative analysis and research on different TES materials are focused on characterization and numerical simulation but less on packed bed TES experiments. This paper evaluates the thermal durabilities of three materials, including sintered ore particles, alumina balls, and rock particles, through thermal cycling tests. Through packed bed heat storage experiments, the energy storage characteristics and thermocline evolution characteristics of three beds under different operating conditions are compared and analyzed. The results indicate that all materials exhibit excellent thermal durabilities. A larger bed voidage and smaller bed heat capacity are beneficial for thermal diffusion in the bed. When reverse charging, the natural convection of air in the bed enhances the convective heat transfer effect, resulting in a higher charging power. The existence of natural convection promotes the mixing of cold air and hot air in the tank, increases the irreversibility of the process, and leads to a significantly lower efficiency in reverse flow compared to that in forward flow. When changing the airflow direction, the system overall exergy efficiencies of SOP, alumina, and rock bed decrease from 74.1 %, 72.4 %, and 77.2 % to 47.0 %, 39.9 %, and 45.8 %, respectively. Regardless of the airflow direction, the smaller the bed voidage and the larger the bed heat capacity, the better the maintenance characteristics of the thermocline.

Investigating novel Mo2X3S (X = Se, Te) materials: probing the influence of chalcogen substitution on electronic, optical, and thermoelectric properties

The excellent thermal performance and adjustable optoelectronic characteristics distinguish the ternary semiconductors. Using the state-of-the-art density functional theory, the optoelectronic, and thermoelectric characteristics of new Mo2X3S (X = Se, Te) ternary chalcogenides are studied. The predicted band gap values with TB-mBJ for Mo2Se3S and Mo2Te3S materials were 1.41 eV and 2.10 eV, respectively. For their possible employment in optoelectronic applications, the components of the complex dielectric function and the vital optical characteristics were calculated and studied. For an increase in the band gap and with the replacement of Se to Te, the peaks in ε 1(ω) shifted to higher energies. Mo2Se3S and Mo2Te3S both show stronger absorption in the UV and visible ranges. Based on the observed peaks in the reflection spectrum, they may used as ultraviolet-reflecting materials with good efficacy. Both Mo2Se3S and Mo2Te3S have positive Seebeck coefficient values, they exhibit p-type conduction. The Mo2Te3S material displays a maximum Seebeck coefficient at about 500 K compared to Mo2Se3S, which leads to a maximum ZT.

Lattice Softening and Band Convergence in GeTe-Based Alloys for High Thermoelectric Performance.

GeTe-based alloys have been studied as promising TE materials in the midtemperature range as a lead-free alternate to PbTe due to their nontoxicity. Our previous study on GeTe1-xIx revealed that I-doping increases lattice anharmonicity and decreases the structural phase transition temperature, consequently enhancing the thermoelectric performance. Our current work elucidates the synergistic interplay between band convergence and lattice softening, resulting in an enhanced thermoelectric performance for Ge1-ySbyTe0.9I0.1 (y = 0.10, 0.12, 0.14, and 0.16). Sb doping in GeTe0.9I0.1 serves a double role: first, it leads to lattice softening, thereby reducing lattice thermal conductivity; second, it promotes a band convergence, thus a higher valley degeneracy. The presence of lattice softening is corroborated by an increase in the internal strain ratio observed in X-ray diffraction patterns. Doping also introduces phonon scattering centers, further diminishing lattice thermal conductivity. Additionally, variations in the electronic band structure are indicated by an increase in density of state effective mass and a decrease in carrier mobility with Sb concentration. Besides, Sb doping optimizes the carrier concentration efficiently. Through a two-band modeling and electronic band structure calculations, the valence band convergence due to Sb doping can be confirmed. Specifically, the energy difference between valence bands progressively narrows upon Sb doping in Ge1-ySbyTe0.9I0.1 (y = 0, 0.02, 0.05, 0.10, 0.12, 0.14, and 0.16). As a culmination of these effects, we have achieved a significant enhancement in zT for Ge1-ySbyTe0.9I0.1 (y = 0.10, 0.12, 0.14, and 0.16) across the entire range of measured temperatures. Notably, the sample with y = 0.12 exhibits the highest zT value of 1.70 at 723 K.

Ultrahigh-response flexible photothermoelectric photodetectors based on a graded Bi2Te3-carbon nanotube hybrid

Photothermoelectric (PTE) detectors can work in a broad band range without using a cooling unit and external bias and therefore have attracted intense research interest. However, the performance of PTE detectors constructed using traditional TE materials has been limited by their poor optical absorption and intrinsic brittleness. We report a flexible graded TE material comprised of Bi2Te3 nanocrystals adsorbed on a single-wall carbon nanotube (SWCNT) network, which has excellent flexibility, high photo-thermal conversion ability and good TE properties. Flexible PTE detectors were constructed, and had an ultrahigh responsivity of 0.71 V/W, a high peak detectivity up to 2.1 × 108 Jones, and a broad response band ranging from the infrared to the terahertz band. The excellent PTE performance of the detectors is attributed to the broadband optical absorption of SWCNTs, the high TE performance of Bi2Te3 nanocrystals, and the graded layer structure of the hybrid.

Ab initio Investigation of quasi-one-dimensional ternary chalcogenides Sr2ZnX3 (X = S, Se, Te) for efficient photovoltaic and thermoelectric applications

The quest for sustainable and renewable energy sources has become a vital global mission. Transition metal chalcogenide materials have garnered significant attention due to their unique low-dimensional physical properties. In this work, we explore the impact of ionic radius in modulating the physical properties of ternary chalcogenides by calculating structural, electronic, optical, and thermoelectric properties of Sr2ZnX3 (X = S, Se, Te) materials using first-principles density functional theory (DFT) as implemented in the WIEN2k program. To evaluate the effect of ionic radius, two novel semiconductors Sr2ZnSe3 and Sr2ZnTe3, were constructed using similar isostructural material Sr2ZnS3. Further optimized structure reveals that the corner-sharing ZnX4 tetrahedra extended along the b-axis confirms the quasi-one-dimensional (Q1D) nature of Sr2ZnX3 materials. Band structure analysis revealed a wide direct bandgap nature with the values of Sr2ZnS3 (3.4 eV), Sr2ZnSe3 (2.8 eV) and Sr2ZnTe3 (1.75 eV), respectively. The lower effective mass of electrons and holes suggests higher carrier mobility and charge recombination rates, vital for photovoltaic applications. The optical properties of the materials are studied in the energy range of 0–10 eV (IR–Vis–UV region). We found that Sr2ZnTe3 material exhibits higher values of dielectric function, absorption coefficient (α≈106 cm−1), refractive index, and lower reflectivity, which indicates its suitability for photovoltaic application. Thermoelectric properties are crucial for assessing material utility in thermoelectric applications, and the study revealed substantial values of the Seebeck coefficient, electrical conductivity, figure of merit (ZT) greater than 2, power factor, and lower electronic thermal conductivity. The studied properties signify Sr2ZnX3 materials as potential candidates for light-emitting semiconductors and thermoelectric applications.

Recent advances in enhancing thermoelectric performance of polymeric materials

The inherent low thermal conductivity, low cost, and flexibility of polymeric materials make them potential candidates for thermoelectric applications. Their eco-friendliness and mechanical flexibility are useful for the design of portable and flexible self-powered electronics. However, the heat-to-electrical power conversion efficiency, also known as the figure-of-merit (ZT), of polymer TE materials is low. Research efforts are in progress to enhance the thermoelectric performance of polymers and to find new kinds of polymer composites. Recent research innovations, such as chemical doping of polymers, development of nanocomposites and hybrid composites, and nanostructuring have significantly changed the thermoelectric properties of the polymeric materials. In this article, we summarize the recent developments and achievements in polymer materials for thermoelectric applications.

The amplification effect of four-phonon scattering in CdX (X=Se, Te): The role of mid-frequency phonons

Recently, CdX (X = Se, Te) materials have garnered notable interest owing to their great application potential for high-efficiency solar cells, fiber optic communication systems, and nanoelectronic devices. The performance of optoelectric devices is significantly influenced by the thermal conductivity. In this study, a combination of machine-learning methods and first-principles calculations is utilized to investigate the phonon thermal transport properties of CdSe and CdTe, as well as to give deep insights into the phonon behavior in heat transfer. It is found that acoustic phonons dominate the lattice thermal conductivity (κ) in CdSe, while optical phonons contribute around 50 % to the κ value in CdTe. There are strikingly strong four-phonon scattering phenomena in both materials, which result in 55 % and 66 % reduction in κ values for CdSe and CdTe, respectively. Further analysis shows that the mid-frequency phonons play an important role in amplifying the four-phonon scattering. Its special frequency positions permit an unusually large number of four-phonon scattering processes to occur and cause large scattering of low-frequency phonons. This mechanism differs from earlier proposed features regarding large acoustic-optical gaps, bunching of acoustic branches and four-phonon Fermi resonance, which implies strong four-phonon anharmonicity. Thus, the present work opens up new prospects in the exploration and design of innovative thermoelectric material, which provides a more thorough understanding of the four-phonon scattering mechanisms in crystalline solids.

Highly Stretchable Thermoelectric Fiber with Embedded Copper(I) Iodide Nanoparticles for a Multimodal Temperature, Strain, and Pressure Sensor in Wearable Electronics

AbstractThermoelectric (TE) fibers have excellent potential for multimodal sensor, which can detect mechanical and thermal stimuli, used in advanced wearable electronics for personalized healthcare system. However, previously reported TE fibers have limitations for use in wearable multimodal sensors due to the following reasons: 1) TE fibers composed of carbon or organic materials have low TE performance to detect thermal variations effectively; 2) TE fibers composed of rigid inorganic materials are not stretchable, limiting their ability to detect mechanical deformation. Herein, the first stretchable TE fiber‐based multimodal sensor is developed using copper(I) iodide (CuI), an inorganic TE material, through a novel fabrication method. The dense CuI nanoparticle networks embedded in the fiber allow the sensor to achieve excellent stretchability (maximum tensile strain of ≈835%) and superior TE performance (Seebeck coefficient of ≈203.6 µV K−1) simultaneously. The sensor exhibits remarkable performances in strain sensing (gauge factor of ≈3.89 with tensile strain range of ≈200%) and pressure sensing (pressure resolution of ≈250 Pa with pressure range of ≈84 kPa). Additionally, the sensor enables independent and simultaneous temperature change, tensile strain, and pressure sensing by measuring distinct parameters. It is seamlessly integrated into a smart glove, demonstrating its practical application in wearable technology.

Thermoelectric performance of newly discovered LiHfPdZ (Z= Al, Ga, and In) quaternary Heusler compounds: A DFT study

Li-based quaternary Heusler LiHfPdZ (Z = Al, Ga, and In) compounds have been investigated for their electronic properties, structural stability, phonon spectra, and thermoelectric performance. Band structure calculations based on Density Functional Theory, show the indirect semiconductor nature of LiHfPdZ (Z = Al, Ga, and In) compounds with band gaps of 0.73 eV, 0.79 eV, and 0.58 eV, respectively. We obtained flat Hf-5d bands (without dispersion) in the vicinity of Fermi energy (EF), resulting in a high value of Seebeck coefficient. The positive values of frequencies in the phonon dispersion curve confirm the dynamic stability of these compounds. The computed elastic properties suggested that the studied compounds are mechanically stable. The calculated values of melting points of this compounds are around 1500 ± 300 K, which ensures the stability of these compounds at high temperatures. We obtained a maximum value of the figure of merit 0.72, 0.68 and 0.67 for LiHfPdAl, LiHfPdGa and LiHfPdIn compounds respectively, which is higher than other Li based QH compounds of same kind i.e. LiHfCoSn (0.59) and LiHfCoGe (0.61) obtained by Singh et al. at same temperature. Overall, a comparatively high and stable value of ZT above 600 K is obtained only in LiHfPdAl, which suggests that it is the most suitable candidate as TE material for high-temperature applications.

Annealing-induced transformation of structural and optical parameters of transparent γ-CuI thin films with superior thermoelectric performance

The synthesis of transparent thermoelectric materials, particularly at low processing temperature possesses a good promise for future power generation by renovating waste heat into electrical energy. The fabrication of invisible thermoelectric module is hindered by limited choices of appropriate p-type transparent thermoelectric materials so far. The present study deals with the growth and characterization of optically transparent p-type copper iodide (γ-CuI) thin films. Thermal annealing (maximum up to 200 °C) was performed to tune the electrical and optoelectronic properties for nurturing the thermoelectric performance. Annealing induced microstructural modifications instigated the preferential crystal growth by regulating the surface morphology. Low thermal conductivity is credited to strong phonon scattering leading to improved thermoelectric performance. Consequently, we attain a record Seebeck coefficient of ∼270 μV/K and power factor of ∼20 μW/(m·K2) that is almost two-order of magnitude higher as compared to conventional p-type transparent TE materials, indicating the potential of transparent γ-CuI thin films regarding its practical applicability in transparent thermoelectric devices.

Wearable thermoelectric cooler encapsulated with low thermal conductivity filler and honeycomb structure for high cooling effect

Thermoelectric coolers (TEC) based on Peltier effect has been widely used in small scale cold storage because of its zero emission, and high efficiency, while wearable thermoelectric coolers (WTEC) for personal temperature management is garnered tremendous scientific attention. For out-of-plane structured WTEC using inorganic TE materials encapsuled in flexibility substrate, on the one hand, encapsulating materials are required to have low thermal conductivity, high reliability and high flexibility, and on the other hand, heat dissipation of devices is required to be lightweight, portable and efficient. For this reason, we propose a composite material synthesised from SiO2 aerogel, hollow glass beads (HGB) and polydimethylsiloxane (PDMS) as a filler, which takes advantage of the low thermal conductivity of (0.094 W/mK) to increase the temperature difference in the encapsulation layer of the device, and moreover performs the fabrication of honeycomb holes, which further reduces the thermal conductivity of the encapsulation layer and at the same time brings a certain degree of compression resistance to the device. Radiative cooling (RC) films synthesised using hexagonal boron nitride (HBN) and PDMS for lowering the temperature of the hot side in outdoor environments without additional energy consumption, providing heat dissipation at the hot side. Honeycomb wearable thermoelectric cooler (HWTEC) proposed in this work deliver high cooling temperature difference of 9.1 °C and 6.5 °C indoor and outdoor through human wear. Our work represents an important step in the development of flexible TE devices and is believed to have promising future applications in personal thermal management, e-skin and smart textiles.

Quantum‐Dot‐Induced Energy Filtering Effect in Organic Thermoelectric Nanocomposites

AbstractThermoelectric (TE) charge transport in organic TE nanocomposite systems is a critical consideration in designing high‐performance TE materials. Here, the relationship between the TE properties and energy structure of conducting polymer/quantum dot (QD) nanocomposites is systematically investigated by developing a potential wall or potential well in poly(3,4‐ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) with CdTe QDs. The added QDs are primarily distributed within the electrically insulating PSS shell and act as stepping stones for charge transport between PEDOT‐rich grains. The embedded QDs generate an energy‐filtering effect, which is induced by both potential wall and potential well states established by the QDs in the PEDOT:PSS films. The induced energy‐filtering effect increases the Seebeck coefficient S with limited loss of electrical conductivity σ, thereby overcoming the TE trade‐off relation S ∝ σ −1/4. The energy‐filtering effect is optimized by carefully controlling the QD size. The PEDOT:PSS/QD nanocomposite containing the smallest QDs exhibits a power factor of 173.8 µW m−1 K−2, which is 80% larger than the value for the pristine PEDOT:PSS film. This work suggests a strategy for designing TE nanocomposites with improved TE performance and emphasizes the importance of fine‐tuning the interfacial energy gap to achieve an effective energy‐filtering effect.

A Waterproof Flexible Paper-Based Thermoelectric Generator for Humidity and Underwater Environments.

A thermoelectric generator (TEG) is one of the important energy harvesting sources for wearable electronic devices, which converts waste heat into electrical energy without any external stimuli, such as light or mechanical motion. However, the poor flexibility of traditional TEGs (e.g., Si-based TE devices) causes the limitations in practical applications. Flexible paper substrates are becoming increasingly attractive in wearable electronic technology owing to their usability, environmental friendliness (disposable, biodegradable, and renewable materials), and foldability. The high water-absorbing quality of paper restricts its scope of application due to water failure. Therefore, we propose a high-performance flexible waterproof paper-based thermoelectric generator (WPTEG). A modification method that infiltrates TE materials into cellulose paper through vacuum filtration is used to prepare the TE modules. By connecting the TE-modified paper with Al tape, as well as a superhydrophobic layer encapsulation, the WPTEG is fabricated. The WPTEG with three P-N modules can generate an output voltage of up to 235 mV at a temperature difference of 50 K, which can provide power to portable electronic devices such as diodes, clocks, and calculators in hot water. With the waterproof property, the WPTEG paves the way for achieving multi-scenario applications in humid environments on human skin.