High-performance Thermoelectric Materials Research Articles

High thermoelectric performances of monolayer GeTe allotropes.

Aiming at finding wide-temperature-zone thermoelectric (TE) materials, five kinds of monolayer GeTe allotropes including the newly designedγ-,δ-, andɛ-GeTe monolayers and the usualα- andβ-GeTe ones are constructed. By using the density functional theory and the nonequilibrium Green's function method, all their electronic properties and TE transport properties are comparatively investigated. It is found that the room-temperature figure of meritZTof theγ-GeTe (ɛ-GeTe) along the armchair (zigzag) direction can amount to 4.5 (3.5), which is further increased to 7.15 (5.91) at 700 K. TheseZTvalues are much higher than the other IV-VI compounds usually withZT < 3, indicating that the armchairγ-GeTe and the zigzagɛ-GeTe we designed here can be used as superior wide-temperature-zone and high-performance TE materials in the temperature range from 300 K to 700 K. Moreover, with the increase of temperature, theZTpeaks will become wider in width and move towards the position of zero chemical potential, which will make the GeTe-based TE devices work at low bias voltages more efficiently. This work should be an important reference on the way to the stage ofZT⩾4, which will motivate more explorations into the high-performance TE materials working in a wider temperature scope.

Enhanced Thermoelectric Performance of SnTe via Introducing Resonant Levels

SnTe has emerged as a non-toxic and environmentally friendly alternative to the high-performance thermoelectric material PbTe, attracting significant interest in sustainable energy applications. In our previous work, we successfully synthesized high-quality SnTe with reduced thermal conductivity under high-pressure conditions. Building on this, in this work, we introduced indium (In) doping to further decrease thermal conductivity under high pressure. By incorporating resonance doping into the SnTe matrix, we aimed to enhance the electrical transport properties while maintaining low thermal conductivity. This approach enhances the Seebeck coefficient to an impressive 153 μVK−1 at 735 K, marking a notable enhancement compared to undoped SnTe. Furthermore, we noted a substantial decrease in total thermal conductivity, dropping from 6.91 to 3.88 Wm−1K−1 at 325 K, primarily due to the reduction in electrical conductivity. The synergistic impact of decreased thermal conductivity and heightened Seebeck coefficient resulted in a notable improvement in the thermoelectric figure of merit (ZT) and average ZT, achieving approximately 0.5 and 0.22 in the doped samples, respectively. These advancements establish Sn1−xInxTe as a promising candidate to replace PbTe in thermoelectric applications, providing a safer and more environmentally sustainable option.

Thermoelectric Performance in Triplet-Ground-State Polymer Intrinsically Boosted by Enhanced Proquinoidal Characteristic.

Over the past decade, polymer thermoelectric materials featuring flexibility, lightness, and bio-friendliness have been paid increasing attention as promising candidates for waste heat recovery and energy generation. For a long time, the dominant approach to optimizing the thermoelectric performance of most organic materials is chemical doping, which, however, is not always ideal for practical applications due to its tendency to involve intricate processing procedure and trigger material and device instability. Currently, the pursuit of single-component neutral thermoelectric materials without exogenous doping presents a compelling alternative. In this work, we designed and synthesized a high-spin polymer material, PBBT-TT, by simultaneously employing thieno[3,4-b]thiophene (TbT) and benzo[1,2-c : 4,5-c']bis[1,2,5]thiadiazole (BBT) units with pronounced proquinoidal characteristics, its analogue, PBBT-T to demonstrate the effect of the TbT unit was also synthesized. The results indicate that because of the enhanced quinoidal resonance, increased spin density and strong intermolecular antiferromagnetic coupling, PBBT-TT exhibits high intrinsic electrical conductivity and Seebeck coefficient, which showcases an outstanding power factor of 26.1 μW m-1 K-2 without doping. This achievement surpasses other neutral organic conjugated polymer and radical conductors, and is even comparable to some typical early-stage doped polymers. Notably, PBBT-TT exhibits remarkable ambient stability, retaining its initial thermoelectric performance over a 120-day period. Our finding demonstrates that modulating the intermolecular spin interactions in open-shell polymers through the introduction of strong proquinoidal units is an effective strategy for the development of doping-free, intrinsically high-performance polymer thermoelectric materials.

High thermoelectric performance in Ag-doped Bi0.5Sb1.5Te3 nanocomposites synthesized via low-temperature liquid phase sintering

In recent years, low-temperature liquid phase sintering (LPS) has emerged as a cost-effectiveness method for designing thermoelectric nanocomposites with reduced lattice thermal conductivity. However, their electrical conductivity often remains suboptimal, limiting the overall figure of merit (ZT). In this study, xwt% Ag/Bi0.5Sb1.5Te3 (x = 0,0.1,0.2,0.3,0.4) nanocomposites are prepared through low-temperature LPS method followed by subsequent annealing. Remarkably, a small amount of silver atoms was doped into the Bi0.5Sb1.5Te3 matrix post-annealing, significantly increasing carrier concentration and improving electrical conductivity. Additionally, residual Ag atoms formed Ag₂Te nanoprecipitates, and lattice defects (including grain boundaries, twin boundaries, dislocations, and lattice distortions) effectively reduced lattice thermal conductivity. The 0.3 wt% Ag/Bi0.5Sb1.5Te3 sample achieved a maximum ZT value of 1.36 at 400 K, double that of the pure Bi0.5Sb1.5Te3 sample, with an average ZT value of 1.17, among the highest reported. This work demonstrates significant potential for synthesizing high-performance thermoelectric materials via low-temperature LPS methods.

Ultralow thermal conductivity and excellent thermoelectric performance in Janus Bi2X2Y (X=Se, Te; Y=S, Se, Te) monolayers induced by suppressed membrane effect

We use density functional theory (DFT) implemented in the Vienna Ab initio Simulation Package (VASP) combined with Boltzmann transport equations to investigate the relationships between the structure, phonon hybridization, transport and thermoelectric properties of two-dimensional (2D) Janus Bi2X2Y (X=Se, Te; Y=S, Se, Te) monolayers. Among them, Janus Bi2Te2S monolayer shows a unique ultralow lattice thermal conductivity (1.09 W·m−1·K−1 at 300 K) and excellent thermoelectric performance. We find that, by suppressing the membrane effect of 2D materials to enable the negative-positive conversion of the Grüneisen parameter of the out-of-plane acoustic (ZA) phonon modes, the three-phonon scattering of the material can be effectively enhanced thereby reducing their lattice thermal conductivity. Besides, we also find the suppression of the membrane effect is highly correlated to the non-orthogonal bond angles. Our results indicate a new path to reduce the lattice thermal conductivity of 2D materials and are meaningful for further theoretical and experimental research on the development of high-performance thermoelectric materials.

Thermal insulation enhanced by the dopant-induced phonon softening discovered in thermoelectric Heusler compounds

Suppression of phonon transports is a key requirement to achieve high thermoelectric performance, which has been often realized by doping an element to enhance the phonon scattering. However, detailed origins behind the dopant-induced low lattice thermal conductivity (κph) have not yet been comprehensively understood. Here, we demonstrate a κph reduction mechanism induced by the phonon softening in the element-doped Fe2VAl thermoelectric Heusler compounds. Inelastic X-ray scattering experiments revealed that overall optical phonons are softened with increasing Ti-doping concentration in marked contrast to the Ta-doped Fe2VAl. By means of photoelectron spectroscopy, we found that the observed phonon softening is originating from the rigid-band shift of the electronic density of states and the consequent deviation of the pseudo-gap position from the Fermi level, which causes the energetic instability of the electronic system. This instability is accompanied by the reduction of the filled bonding states, giving rise to the phonon softening. This mechanism of κph reduction caused by the close correlation between electronic and phononic systems will shed new light on achieving low-κph and thereby developing unconventional high-performance thermoelectric materials.

Excellent thermoelectric performance in alkali metal phosphides M3P (M = Na and K) with phonon-glass electron-crystal like behaviour.

Identifying ideal thermoelectric materials presents a formidable challenge due to the intricate coupling relationship between thermal conductivity and power factor. Here, based on first-principles calculations, along with self-consistent phonon theory and the Boltzmann transport equation, we theoretically investigate the thermoelectric properties of alkali metal phosphides M3P (M = Na and K). The evident 'avoided crossing' phenomenon indicates the phonon glass behavior of M3P (M = Na and K). Due to the strong lattice anharmonicity induced by alkali metal elements, accounting for quartic anharmonic corrections, the lattice thermal conductivities of Na3P and K3P at room temperature are merely 0.25 and 0.12 W m-1 K-1, respectively. Furthermore, the high degeneracy and 'pudding-mold-type' band structure lead to high p-type PF in M3P (M = Na and K). At 300 K, the p-type power factors (PF) of Na3P and K3P can reach 3.90 and 0.80 mW mK-2, respectively. The combination of ultralow κL and high PF leads to excellent thermoelectric figure of merit (ZT) values of 1.70 (3.38) and 1.18 (2.13) for p-type Na3P and K3P under optimal doping concentration at 300 K (500 K), respectively, surpassing traditional thermoelectric materials. These findings demonstrate that M3P (M = Na and K) exhibits behavior similar to phonon-glass electron crystals, thereby indicating a direction for the search for high-performance thermoelectric materials.

Flexible and air-stable n-type oleylamine/carbon nanotube hybrid yarns for high-performance wearable thermoelectric generators

Wearable thermoelectric generators (TEGs), envisioned to harness the temperature gradient (ΔT) between the human body and the environment into electricity, hold great promise for powering wearable electronics. However, their practical application has been hampered by the scarcity of flexible n-type thermoelectric (TE) materials boasting both high performance and long-term air stability. Here, we introduce a significant advancement by developing an n-type TE material through immersing carbon nanotube yarn (CNTY) into an oleylamine (OAm)/ethanol solution, followed by drying under atmospheric conditions. The resulting OAm/CNTY exhibits a Seebeck coefficient of -80.48 μV K-1, an electrical conductivity of 1353.18 S cm-1 and a power factor of 876.25 μW m-1 K-2, all while exhibiting exceptional mechanical flexibility. Notably, this hybrid yarn maintains stable n-type behavior even after enduring exposure to air for over 370 days, surpassing previous n-type TE materials based on CNT fibers and CNTY. Leveraging this advancement, we construct a prototype wearable TEG by alternately embroidering pristine p-type CNTY and n-type OAm/CNTY into a polyester spacer fabric, electrically connecting them in series using conductive silver paint. The resulting wearable TEG, featuring with 150 p-n couples, yields an output voltage of 705.94 mV and a maximum output power of 44.34 μW at a ΔT of 40 K. This groundbreaking work opens new avenues for the development of high-performance, air-stable, and flexible n-type TE material, ushering in a new era for wearable TEGs.

Alloy scattering to optimize carrier and phonon transport properties in PbBi2S4 thermoelectric

Ternary PbBi2S4 compound with crustal S-rich element and low lattice thermal conductivity is considered as a potential thermoelectric candidate. However, its inferior thermoelectric properties are rooted in the low electrical transport performance. Generally, enhancing electrical transport performance (power factor, PF) primarily entails optimizing the interdependent relationship between carrier mobility μ (linked to electrical conductivity σ) and effective mass m* (related to Seebeck coefficient S). In this work, we introduce the strategy of alloy scattering to independently enhance S without weakening μ and simultaneously reduce thermal conductivity, leading to a synergetic optimization of electron and phonon in PbBi2S4 thermoelectric. Heavy Sn alloying in PbBi2S4 presents uniform and orderly distribution on Pb sites as unclosed by the atomic-scale crystal structure observation. These massive Sn atom serves as scattering centers and turns the electron scattering mechanism to be dominated by alloy scattering, thus resulting in a ∼ 33% increment of S in Pb0.6Sn0.4Bi2S4. Meanwhile, Sn alloying aggravates phonon scattering further lowering lattice thermal conductivity and reaching an extremely low value of 0.34 W·m–1·K–1 at 773 K. Finally, a maximum zT of 0.68 at 773 K is obtained in Pb0.6Sn0.4Bi2S4, which is ∼ 45% higher than the pristine matrix. This study proves that the strategy of alloy scattering is effective in improving overall electrical transport properties as well as reducing lattice thermal conductivity, which paves a new way to develop high-performance thermoelectric materials.

The Influence of Molecular Weights on Dispersion and Thermoelectric Performance of Alkoxy Side-Chain Polythiophene/Carbon Nanotube Composite Materials.

In the development of wearable electronic devices, the composite modification of conductive polymers and single-walled carbon nanotubes (SWCNTs) has become a burgeoning research area. This study presents the synthesis of a novel polythiophene derivative, poly(3-alkoxythiophene) (P3(TEG)T), with alkoxy side chains. Different molecular weight variants of P3(TEG)T (P1-P4) were prepared and combined with SWCNTs to form composite materials. Density functional theory (DFT) calculations revealed a reduced bandgap for P3(TEG)T. Raman spectroscopy demonstrated π-π interactions between P3(TEG)T and SWCNTs, facilitating the dispersion of single-walled carbon nanotubes and the formation of a continuous conductive network. Among the composite films, P4/SWCNTs-0.9 exhibited the highest thermoelectric performance, with a power factor (PF) value of 449.50 μW m-1 K-2. The fabricated flexible thermoelectric device achieved an output power of 3976.92 nW at 50 K, with a tensile strength of 59.34 MPa for P4/SWCNTs. Our findings highlight the strong interfacial interactions between P3(TEG)T and SWCNTs in the composite material, providing an effective charge transfer pathway. Furthermore, an improvement in the tensile performance was observed with an increase in the molecular weight of the polymer used in the composite, offering a viable platform for the development of high-performance flexible organic thermoelectric materials.

A new strategy to simultaneously optimize Seebeck coefficient and electrical conductivity of PEDOT:PSS polymer via L-ascorbic acid

PEDOT:PSS flexible thermoelectric materials are promising for future wearable continuous power support, but it remains challenging due to low power factor. Herein, we propose a “one-stone-two-birds” strategy using L-ascorbic acid as the reductant in synthesis of tellurium nanorods and separating agent in in-situ removing PSS chains. L-ascorbic acid reduces Te4+ to Te, supplying inorganic thermoelectric materials with high Seebeck coefficient as fillers to significantly increase the Seebeck coefficient value of PEDOT:PSS. Meanwhile, L-ascorbic acid separates PSS chains from PEDOT chains, resulting in the increase of electrical conductivity at room temperature by ∼360 % due to structure transformation from benzoid structure to the quinoid structure in PEDOT. As a result, the power factor of optimal PEDOT:PSS with Te fillers and L-ascorbic acid treatment is improved significantly by ∼100 times as compared to that of pristine PEDOT:PSS. Finally, a prototype wearable thermoelectric generator was assembled by 18 legs of Te/PEDOT:PSS composites, which demonstrates a high power density of 2.3 μW·cm−2 with good mechanical stability, flexibility and durability. The present study offers a new strategy for rational design of high-performance flexible thermoelectric materials from PEDOT:PSS.

Thermoelectric Property Enhancement of Tellurium Nanowires by Surface Passivation.

The pursuit of high-performance thermoelectric materials is of paramount importance in addressing energy sustainability and environmental concerns. Here, we explore the multifaceted impact of sulfur passivation in the matrix of tellurium nanowires (TeNWs), encompassing environmental control, thermoelectric properties, and charge carrier mobility. In this study, we present the facile production of TeNWs using an aqueous solution synthesis approach. The synthesized TeNWs were subsequently subjected to surface modification involving sulfur moieties. Our findings demonstrate that sulfur passivation not only effectively safeguards the nanowires from environmental degradation but also significantly augments their thermoelectric properties. Notably, the highest recorded values were achieved at 560 K for passivated tellurium nanowires, exhibiting a Seebeck coefficient of 246 μV/K, an electrical conductivity of 14.2 S/cm, and power factors of 86.7 μW/m-K2. This strategy presents a promising avenue for the development of advanced thermoelectric materials for applications in energy harvesting, waste heat recovery, and sustainable energy conversion technologies.

Isomers of n-Type Poly(thiophene-alt-co-thiazole) for Organic Thermoelectrics.

n-Type polythiophene represents a promising category of n-type polymer thermoelectric materials known for their straightforward structure and scalable synthesis. However, n-type polythiophene often suffers from a twisted backbone and poor stacking property when introducing high-density electron-withdrawing groups for a lower lowest unoccupied molecular orbital (LUMO) level, which is considered to be beneficial for n-doping efficiency. Herein, we developed two isomers of polythiophene derivatives, PTTz1 and PTTz2, by inserting thiazole units into the polythiophene backbone composed of thieno[3,4-c]pyrrole-4,6-dione (TPD) and thiophene-3,4-dicarbonitrile (2CNT). Although PTTz1 and PTTz2 share a similar polymer skeleton, they differ in thiazole configuration, with the nitrogen atoms of the thiazole units oriented toward TPD and 2CNT, respectively. The insertion of thiazole units significantly planarizes the polythiophene backbone while largely preserving low LUMO levels. Notably, PTTz2 exhibits a more coplanar backbone and closer π-stacking compared to PTTz1, resulting in a greatly enhanced electron mobility. Both PTTz1 and PTTz2 can be easily n-doped due to their deep LUMO levels. PTTz2 demonstrates superior thermoelectric performance, with an electrical conductivity of 50.3 S cm-1 and a power factor of 23.8 μW m-1 K-2, which is approximately double that of PTTz1. This study highlights the impact of the thiazole unit on n-type polythiophene derivatives and provides valuable guidelines for the design of high-performance n-type polymer thermoelectric materials.

High-Performance SnTe Thermoelectric Materials Enabled by the Synergy of Band Convergence and Phonon Scattering.

SnTe, an environmentally friendly thermoelectric material, has garnered widespread scholarly interest owing to its lead-free nature; however, its intrinsic thermoelectric performance is constrained by a relatively low Seebeck coefficient and an extremely high lattice thermal conductivity. In this investigation, we employ the alloying of Ge and AgSbTe2 to enhance the zT value of SnTe. The study found that Ge, Ag, and Sb can effectively enhance the Seebeck coefficient and power factor of SnTe by utilizing band convergence. At the same time, a multitude of point defects induce phonon scattering, consequently decreasing the lattice thermal conductivity of SnTe. Collectively, these synergistic effects result in Sn0.75Ge0.25Te-15% AgSbTe2 achieving its highest zT value of 1.28 at 823 K, with an average zT value of 0.77 between 400 and 823 K. Such high zT values of the SnTe-based thermoelectric material provide the potential for applications in high-performance solid-state thermoelectric devices.

Excellent thermoelectric performance of Fe2NbAl alloy induced by strong crystal anharmonicity and high band degeneracy

Full-Heusler alloys with earth-abundant elements exhibit high mechanical strength and favorable electrical transport behavior, but their high intrinsic lattice thermal conductivity limits potential thermoelectric application. Here, the thermoelectric transport properties of Fe-based Full-Heusler Fe2MAl (M = V, Nb, Ta) alloys are comprehensively investigated utilizing density functional theory. The results suggest that Fe2NbAl exhibits exceptionally low lattice thermal conductivity due to low phonon velocities and weakly bound Nb atoms. In Fe2NbAl, the underbonding of the Nb atoms leads large Grüneisen parameters and high anharmonic scattering rates of low-frequency acoustic phonon. Meanwhile, the high band degeneracy and large electrical conductivity lead to a maximum p-type power factor of 255.6 μW·K−2·cm−1 at 900 K. The combination of low lattice thermal conductivity and favorable electrical transport properties leads a maximum p-type dimensionless figure of merit of 1.7. Our work indicates Fe2NbAl, as a low-cost, environmentally friendly, is a potential high-performance p-type thermoelectric material.

(Digital Presentation) Synergistic Enhancement of Thermoelectric Performance through One-Dimensional Hybrid Nanocomposites: Wrapped Nickel Oxide-Decorated Multi-Walled Carbon Nanotubes with Polypyrrole

Given the drawbacks of organic materials’ thermoelectric (TE) conversion efficiency, an approach has been made in this study to synthesize a hybrid organic-inorganic material based on polypyrrole (PPy), multi-walled carbon nanotubes (MWCNTs) and nickel oxide nanoparticles (NiO). The nanocomposite is formed through three steps: MWCNTs functionalization via diazonium salt grafting of 5-amino-1,2,3-benzene tricarboxylic acid; in situ generation on their surfaces of NiO nanoparticles with a homogenous distribution; the chemical polymerization of pyrrole using methyl orange as templating and dopant to wrap the MWCNTs-(COOH)3-NiO. To explore the structural and physical properties of the fillers and the nanocomposites, X-ray diffraction (XRD), Transmission electron microscopy (TEM), Raman spectrometer, Fourier transform infrared spectroscopy (FTIR), and X-ray photoelectron spectroscopy (XPS) were used. Thereby investigating the electrical conductivity (𝜎), Seebeck coefficient (S) and thermal conductivity (κ) at room temperature, a promising improvement was observed in PPy-MWCNTs-(COOH)3-NiO compared to pure PPy. The observed enhancements in TE properties (ZTPPy-MWCNTs-(COOH)3-NiO = 1.51×10-2) are attributed to the presence of NiO, which acts as a dopant and improves the charge carrier density in the nanocomposite; this result could be increased at higher temperatures. Overall, these results demonstrate the potential of our approach for developing high-performance TE materials with applications in energy harvesting and waste heat recovery. Furthermore, this approach offers the potential for scalability and reproducibility, making it a promising method for large-scale fabrication of high-performance composites. Figure 1

Compositional tuning of weighted mobility and phonon scattering in Ti(S1-xSex)2: a strategy for high-performance thermoelectric materials

Compositional tuning of weighted mobility and phonon scattering in Ti(S1-xSex)2: a strategy for high-performance thermoelectric materials

Enhanced thermoelectric properties for eco-friendly CaTiO3 by band sharpening and atomic-scale defect phonon scattering

CaTiO3-based compounds have emerged as a promising thermoelectric material, renowned for their environmentally benign, thermally stable, and cost-efficient merits. Non-etheless, the pristine CaTiO3 manifests inherently low electronic transport properties. Herein, the thermoelectric properties of Ca1-xDyxTiO3 (x = 0, 0.05, 0.10, 0.15, 0.20) compounds are systematically investigated. The electrical transport properties are markedly enhanced by synergistic optimization of the carrier concentration, mobility, and density-of-states effective mass. Density functional theory results demonstrate that the conduction band tends to be sharper and that the lighter band participates in carrier transport after Dy doping. The large discrepancy in atomic mass results in considerable mass fluctuations, which give rise to intense phonon scattering. Benefitting from the modulated band structure and reduced thermal conductivity, the highest thermoelectric figure of merit (ZT) of 0.31 is achieved at 1073 K, enhanced by 287.5% in contrast with pristine CaTiO3 (ZTmax = 0.08). The defect and energy band modulation strategies proposed to optimize thermoelectric performance are applicable to other thermoelectric materials. This investigation inspires the exploration of high-performance and eco-friendly high-temperature thermoelectric material.

Enhancement of thermoelectric properties of p-type bismuth telluride bulk composites with Ag-TiO2 nano particles via spray coating and hot deformation process

We aimed to enhance p-type Bi0.4Sb1.6Te3.4 (BST) composite's thermoelectric (TE) properties by minimizing thermal conductivity through hierarchical phonon scattering via nano Ag-coated TiO2 (Ag/TiO2). Hot deformation (HD) was employed to induce multi-scale microstructures in these high-performance p-type TE materials, affecting electrical and thermal transport properties through improved textures and donor-like effects. Our optimization strategy included creating grain boundaries, multiple phonons scattering centers, and introducing high-density lattice defects, significantly reducing lattice thermal conductivity. The combined effects led to a noticeable improvement in the figure of merit (zT) across the temperature range, with all TE parameters measured along the in-plane direction. In the case of the hot-deformed Bi0.4Sb1.6Te3.4 alloy, the maximum zT reached 1.31 at 350 K, while the average zT (zTavg) was 1.17 in the range of 300–400 K, suggesting promising potential for near room temperature TE power generation and solid-state cooling.

Enhanced thermoelectric properties of 3D printed Bi2Te2.7Se0.3 by atomic interface engineering

The performance of n-type Bi2Te3 materials prepared by selective laser melting (SLM) 3D printing technology tends to be lower than p-type materials. Herein, a bottom-up interface engineering strategy based on Atomic Layer Deposition (ALD) is presented to improve the properties of n-type Bi2Te2.7Se0.3 (BTS) materials prepared by SLM. To validate this strategy, a ZnO ultrathin layer was applied to the grain boundaries of BTS, synergistically optimizing carrier/phonon transport. In terms of electrical transport, the energy filtering effect triggered by the constructed ZnO/BTS interface effectively enhances the Seebeck coefficient of the Bi2Te3 material printed by SLM, substantially increasing the power factor. Additionally, the high thermal stability of the ALD-deposited ZnO ultrathin layer effectively suppresses the volatilization of Te in BTS, regulating the carrier concentration. Regarding thermal transport properties, the multiscale defects introduced by the non-equilibrium solidification process during SLM printing cause effective phonon scattering across a wide frequency range, which in turn reduces the thermal conductivity of the material. Atomic-level interface modification in SLM-printed BTS enhanced the ZT value to 1.25. Exploiting this superior thermoelectric performance, a thermoelectric module was constructed. It demonstrated a conversion efficiency of 5.7 % with a temperature difference of 200 K, comparable to the advanced Bi2Te3-based thermoelectric modules. The integration of an ALD interface modification strategy with SLM technology has not only demonstrated potential applications in Bi2Te3-based thermoelectric material development, but also bears significant importance for the accelerated advancement of high-performance thermoelectric materials in other systems.