Performance Robustness Navigates the Development of Natural Mineral‐Based Thermoelectrics

ABSTRACT Current high‐performance thermoelectric (TE) materials commonly require high‐purity raw materials, delicately designed composition, and elaborate synthesis procedures. Herein, based on a high‐throughput theoretical investigation, we propose a general screen principle of searching compounds with large effective mass and low lattice thermal conductivity to realize robust TE performance upon impurities and defects, which substantially save the energy and time consumptions for large‐scale applications. Taking Cu 12 Sb 4 S 13 , which is predicted to exhibit the strongest performance robustness, as a prototypical example, we demonstrate that the composition and microstructure discrepancies only lead to slight fluctuation on its zT values. Using abundant stibnite and tetrahedrite minerals combining with industrial grade Cu and S powder (99%) as raw materials, a maximum zT value of ∼0.8 at 723 K and a ZT ave of 0.5 in the temperature range of 323–723 K can be achieved dispensing with elaborate chemical doping procedure. Comparing with those prepared using analytical‐grade pure elements, the TE performance can be remained by 80%, while the energy consumption is sharply reduced by more than 85%. These findings unveil the critical role and physical origin of performance robustness in TEs, which guides the development of natural mineral‐based compounds for practical TE applications.