Abstract Solid‐state bismuth telluride‐based thermoelectric devices enable the generation of electricity from temperature differences and have been commercially applied in various fields. However, in many scenarios, the surface of the heat source is not flat. Therefore, it is crucial to develop flexible thermoelectric materials and devices to efficiently utilize heat sources and expand their applications. Compared with organic thermoelectric materials and devices, inorganic flexible thermoelectric materials and devices have much higher thermoelectric performance and stability. Considering the rapid development in this research field, we carefully summarize the design principles, structures, and thermoelectric properties of inorganic flexible materials and their devices reported in the recent 3 years, including sulfides, selenides, tellurides, and composite materials designed based on these inorganics. The structural designs of flexible thermoelectric devices based on micro‐sized bulk materials are also carefully summarized. Additionally, we overview the mechanical stability and methods for reducing internal resistance for designs of inorganic flexible thermoelectric devices. In the end, we provide outlooks on future research directions for inorganic flexible thermoelectric materials and devices. This review will help guide thermoelectric researchers, beginners, and students. 

Advances in flexible inorganic thermoelectrics

Quasi-one-dimensional bulk thermoelectrics

Low-temperature thermoelectric (TE) materials and devices gaining traction in the field of heat management for optical communication chips and integrated circuits, owing to their exceptional qualities such as high response speed, precise temperature control, and absence of mechanical moving parts. However, despite several decades of research on TE materials, the focus has primarily been on temperatures above 300 K, and enhancing the performance of low-temperature TE materials remains a huge challenge. With the recent emergence of competitive low-temperature TE materials, such as SnSe, α-MgAgSb, Mg3Bi2, etc., it has become imperative to extract universal strategies to improve the performance of TE materials at low temperatures. Consequently, this review aims to comprehensively summarize the working mechanisms of TE devices and uncover the common requirement of high electrical transport for TE material at low temperatures. Additionally, we introduce the fundamental theory and improvement strategies of low-temperature electrical properties. Furthermore, we overview the research progress of low-temperature thermoelectric materials and propose the potential research efforts of single crystal and polycrystal with high texture degrees to further enhance their performance. 

Low-Temperature Thermoelectric Materials and Applications

Layered materials exhibit potential for thermoelectric applications, which are reliant on microstructural texture for high performance. In this work, we present layered crystal stacking hot deformation (LCSHD), which leverages anisotropic crystal structures to induce rapid texture formation, leading to high thermoelectric performance. Taking n-type bismuth telluride (Bi2Te3) as a representative, the LCSHD method contributed to a record-high power factor (PF) of 45 μW cm−1 K−2 in polycrystals. Additionally, the dislocation tangle and low-angle grain boundary can be found in the LCSHD sample, producing low lattice thermal conductivity and a remarkable ZT value of 1.2. Benefiting from a reliable high ZT, we prepared a seven-pair Bi2Te3-based module, which displayed an extraordinary conversion efficiency of 6.4% and competitive refrigeration performance. In addition, a significant improvement of ZT value in other layered materials, including SnSe2 and SnSe, was also demonstrated. Our finding offers novel avenues for texture engineering, facilitating the design of high-performance layered thermoelectric materials. 

General design of high-performance and textured layered thermoelectric materials via stacking of mechanically exfoliated crystals

Recent experiments reported an antisymmetric planar Hall effect, where the Hall current is odd in the in plane magnetic field and scales linearly with both electric and magnetic fields applied. Existing theories rely exclusively on a spin origin, which requires spin-orbit coupling to take effect. Here, we develop a general theory for the intrinsic planar Hall effect (IPHE), highlighting a previously unknown orbital mechanism and connecting it to a band geometric quantity-the anomalous orbital polarizability (AOP). Importantly, the orbital mechanism does not request spin-orbit coupling, so sizable IPHE can occur and is dominated by an orbital contribution in systems with weak spin-orbit coupling. Combined with first-principles calculations, we demonstrate our theory with quantitative evaluation for bulk materials TaSb_{2}, NbAs_{2}, and SrAs_{3}. We further show that AOP and its associated orbital IPHE can be greatly enhanced at topological band crossings, offering a new way to probe topological materials.

Orbital Origin of the Intrinsic Planar Hall Effect.

A quasi-one-dimensional bulk thermoelectrics with high performance near room temperature.

In transition-metal dipnictides TmPn2 ( Tm = Ta and Nb; Pn = P, As, and Sb), the origin of extremely large magnetoresistance (XMR) is yet to be studied by the direct visualization of the experimental band structures. Here, using angle-resolved photoemission spectroscopy, we map out the three-dimensional electronic structure of NbAs2. The open-orbit topology contributes to a non-negligible part of the Fermi surfaces (FSs), like that of the isostructural compound MoAs2, where the open FS is proposed to likely explain the origin of XMR. We further demonstrate the observation of open characters in the overall FSs of W2As3, which is also a XMR semimetal with the same space group of C12/ m1 as the TmPn2 family and MoAs2. Our results suggest that the open-orbit FS topology may be a shared feature between XMR materials with the space group of C12/ m1 and, thus, could possibly play a role in determining the corresponding XMR effect together with the electron–hole compensation.

Electronic structure and open-orbit Fermi surface topology in isostructural semimetals NbAs2 and W2As3 with extremely large magnetoresistance


 We report a comprehensive study on a layered-structure compound of NaZn4As3, which has been predicted to be an ideal topological semimetal (TSM) candidate. It is found that NaZn4As3 undergoes a structural transformation from high temperature rhombohedral to a low temperature monoclinic phase. The electric resistivity exhibits a metal-to-insulator-like transition at around 100 K, and then develops a plateau at low temperature, which might be related to the protected topologically conducting surface states. Our first-principles calculation confirms further that NaZn4As3 is a topological insulator (TI) for both different phases rather than a previously proposed TSM. The Hall resistivity reveals that the hole carriers dominate the transport properties for the whole temperature range investigated. Furthermore, an obvious kink possibly associated to the structure transition has been detected in thermopower around ~ 170 K. The large thermopower and moderate κ indicate that NaZn4As3 and /or its derivatives can provide a good platform for optimizing and studying the thermoelectric performance.

Structural phase transition and transport properties in the topological material candidate NaZn4As3

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A quasi-one-dimensional bulk thermoelectrics with high performance near room temperature.

Electronic structure and open-orbit Fermi surface topology in isostructural semimetals NbAs2 and W2As3 with extremely large magnetoresistance

Structural phase transition and transport properties in the topological material candidate NaZn4As3