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.

层状材料具有热电应用的潜力，其高性能依赖于微结构纹理。在这项工作中，我们提出了层状晶体堆叠热变形（LCSHD），它利用各向异性晶体结构来诱导快速织构形成，从而实现高热电性能。以n型碲化铋（Bi ₂ Te ₃ ）为代表，LCSHD方法在多晶中实现了45 μW cm ^-1 K ^-2的创纪录高功率因数（ PF ） 。此外，在 LCSHD 样品中可以发现位错缠结和小角度晶界，从而产生较低的晶格热导率和高达 1.2 的显着ZT值。受益于可靠的高ZT ，我们制备了七对Bi ₂ Te ₃基模块，其表现出6.4%的非凡转换效率和具有竞争力的制冷性能。此外，还证明了其他层状材料（包括SnSe ₂和SnSe）的ZT值的显着改善。我们的发现为纹理工程提供了新颖的途径，促进了高性能层状热电材料的设计。