Thermoelectric refrigeration is one of the mature techniques used for cooling applications, with the great advantage of miniaturization over traditional compression refrigeration. Due to the anisotropic thermoelectric properties of n‐type bismuth telluride (Bi2Te3) alloys, these two common methods, including the liquid phase hot deformation (LPHD) and traditional hot forging (HF) methods, are of considerable importance for texture engineering to enhance performance. However, their effects on thermoelectric and mechanical properties are still controversial and not clear yet. Moreover, there has been little documentation of mechanical properties related to micro‐refrigeration applications. In this work, the above‐mentioned methods are separately employed to control the macroscopic grain orientation for bulk n‐type Bi2Te3 samples. The HF method enabled the stabilization of both composition and carrier concentration, therefore yielding a higher quality factor to compare with that of LPHD samples, supported by DFT calculations. In addition to superior thermoelectric performance, the HF sample also exhibited robust mechanical properties due to the presence of nano‐scale distortion and dense dislocation, which is the prerequisite for realizing ultra‐precision machining. This work helps to pave the way for the utilization of n‐type Bi2Te3 for commercial micro‐refrigeration applications.

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/advs.202206395

Design of N‐Type Textured Bi2Te3 with Robust Mechanical Properties for Thermoelectric Micro‐Refrigeration Application

Synergistically Enhanced Thermoelectric and Mechanical Performance of Bi2te3 Via Industrial Scalable Hot Extrusion Method for Cooling and Power Generation Applications

Defect engineering is an effective method for tuning the performance of thermoelectric materials and shows significant promise in advancing thermoelectric performance. Given the rapid progress in this research field, this Review summarizes recent advances in the application of defect engineering in thermoelectric materials, offering insights into how defect engineering can enhance thermoelectric performance. By manipulating the micro/nanostructure and chemical composition to introduce defects at various scales, the physical impacts of diverse types of defects on band structure, carrier and phonon transport behaviors, and the improvement of mechanical stability are comprehensively discussed. These findings provide more reliable and efficient solutions for practical applications of thermoelectric materials. Additionally, the development of relevant defect characterization techniques and theoretical models are explored to help identify the optimal types and densities of defects for a given thermoelectric material. Finally, the challenges faced in the conversion efficiency and stability of thermoelectric materials are highlighted and a look ahead to the prospects of defect engineering strategies in this field is presented. 

Defect Engineering Advances Thermoelectric Materials

Multi-scale Hierarchical Microstructure Modulation Towards High Room Temperature Thermoelectric Performance in n-Type Bi2Te3-based Alloys

N-type Bi2Te2.7Se0.3 (BTS) alloy has relatively low thermoelectric performance as compared to its p-type counterpart, which restricts its widespread applications. Herein, we designed and prepared a novel composite system, which consists of an n-type BTS matrix incorporated with both inorganic and organic nanoinclusions. The results indicate that the thermopower of the composite samples can be enhanced by more than 19% upon incorporating inorganic nanophase AgBi3S5 (ABS) due to the energy-dependent carrier scattering, which ensures a high power factor. On the other hand, further incorporation of organic nanophase polypyrrole (PPy) can drastically reduce its lattice thermal conductivity owing to the strong scattering of mid- and low-frequency phonons at these nanoinclusions. As a result, high figures of merit ZTmax = 1.3 at 348 K and ZTave = 1.17 (300-500 K) are achieved with improved mechanical properties in BTS-based composites incorporated with 1.5 wt % ABS and 0.5 wt % PPy, demonstrating that the incorporation of both inorganic and organic nanoinclusions is an effective way to improve its thermoelectric performance.

High Thermoelectric Performance of n-type BiTeSe-Based Composites Incorporated with Both Inorganic and Organic Nanoinclusions.

It is known that Yb-filled skutterudite with excellent thermoelectric performance is promising for a power generation device in the intermediate temperature region. Here we created a new approach to obtain nanostructured materials by adding Si to Co-overstoichiometric Yb-filled skutterudite through high-energy ball milling, which embedded bottom-up formed CoSi2 nanoparticles into grain-refining Yb0.25Co4Sb12, synergistically resulting in the enhanced thermoelectric properties and room-temperature hardness. On one hand, the abundant grain boundaries and phase interfaces effectively blocked the propagation of medium-low frequency phonons, resulting in a lower lattice thermal conductivity. On the other hand, phase interfaces barrier nicely screened a portion of low-energy electrons, leading to an improved power factor. As a result, an enhanced peak ZT value of ∼1.43 at 823 K and a promising average ZT of ∼1.00 between 300 and 823 K were achieved in the Yb0.25Co4Sb12/0.05CoSi2 sample. Meanwhile, such nanostructures also enhanced the hardness through the collective contributions of second phase and fine grain strengthening, which made skutterudite more competitive in practical application.

Enhanced Thermoelectric Performance of Yb-Filled Skutterudite with Bottom-Up Formed CoSi2 Nanoparticles.

Sustained thermoelectric efforts have concentrated on the enhancement of conversion efficiency of power generators, while simultaneously achieving high output power continues to lag. Specifically, the highest output power density of emerging Mg‐based modules reported so far is only half of that of commercial Bi2Te3‐based, mainly due to the low power factor of MgAgSb. Herein, homogenously distributed MgCuSb in situ nanoprecipitates in the MgAgSb matrix effectively optimized carrier concentration due to the effect of carrier injection from the metal–semiconductor Ohmic contact. As a result, a record‐high average power factor of 27.2 µW cm−1 K−2 is obtained in MgCu0.1Ag0.87Sb0.99 composite within the temperature range of 300–550 K, which is much higher than ever reported values of MgAgSb system. Benefiting from the combination of the optimized average power factor of p‐leg and low interface resistivity, a fabricated eight‐pair MgCu0.1Ag0.87Sb0.99/Mg3.2Bi1.5Sb0.5 module demonstrates an unprecedently high output power density of 2.9 W cm−2 under a temperature difference of 300 K, outperforming all low‐temperature advanced thermoelectric modules. Meanwhile, a competitive conversion efficiency of 7.65% is obtained simultaneously. The work significantly advances high‐power thermoelectric applications of Mg‐based modules in the field of low‐temperature sustainable energy harvesting.

Semiconductor–Semimetal Composite Engineering Enabling Record‐High Thermoelectric Power Density for Low‐Temperature Energy Harvesting

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Design of N‐Type Textured Bi2Te3 with Robust Mechanical Properties for Thermoelectric Micro‐Refrigeration Application

Enhanced Thermoelectric Performance of Yb-Filled Skutterudite with Bottom-Up Formed CoSi2 Nanoparticles.

Semiconductor–Semimetal Composite Engineering Enabling Record‐High Thermoelectric Power Density for Low‐Temperature Energy Harvesting