All-SnTe-Based Thermoelectric PowerGeneration Enabled by Stepwise Optimization of n‑Type SnTe

The practical application of thermoelectric devices requires both high-performance n-type and p-type materials of the same system to avoid possible mismatches and improve device reliability. Currently, environmentally friendly SnTe thermoelectrics have witnessed extensive efforts to develop promising p-type transport, making it rather urgent to investigate the n-type counterparts with comparable performance. Herein, we develop a stepwise optimization strategy for improving the transport properties of n-type SnTe. First, we improve the n-type dopability of SnTe by PbSe alloying to narrow the band gap and obtain n-type transport in SnTe with halogen doping over the whole temperature range. Then, we introduce additional Pb atoms to compensate for the cationic vacancies in the SnTe–PbSe matrix, further enhancing the electron carrier concentration and electrical performance. Resultantly, the high-ranged thermoelectric performance of n-type SnTe is substantially optimized, achieving a peak <i>ZT</i> of ∼0.75 at 573 K with a high average <i>ZT</i> (<i>ZT</i>_ave) exceeding 0.5 from 300 to 823 K in the (SnTe_0.98I_0.02)_0.6(Pb_1.06Se)_0.4 sample. Moreover, based on the performance optimization on n-type SnTe, for the first time, we fabricate an all-SnTe-based seven-pair thermoelectric device. This device can produce a maximum output power of ∼0.2 W and a conversion efficiency of ∼2.7% under a temperature difference of 350 K, demonstrating an important breakthrough for all-SnTe-based thermoelectric devices. Our research further illustrates the effectiveness and application potential of the environmentally friendly SnTe thermoelectrics for mid-temperature power generation.