TY - JOUR
T1 - Triple-Conduction-Band Activation Enables High Out-of-Plane Thermoelectric Efficiency in n-type SnS Crystals
AU - Hu, Yixuan
AU - Bai, Shulin
AU - Gao, Dezheng
AU - Su, Lizhong
AU - Shi, Haonan
AU - Gao, Tian
AU - Zhan, Shaoping
AU - Liu, Shan
AU - Liu, Shibo
AU - Li, Yichen
AU - Chen, Pengpeng
AU - Liu, Rong
AU - Qin, Bingchao
AU - Zhao, Li Dong
N1 - Publisher Copyright:
© 2025 American Chemical Society
PY - 2025/12/3
Y1 - 2025/12/3
N2 - The increasing interest for high-performance and earth-abundant thermoelectrics has motivated attention toward sulfide-based compounds. Among them, tin sulfide (SnS) has emerged as a promising candidate, especially in its p-type form. However, progress in n-type SnS has been hindered by poor electrical transport. In this study, Se and Pb are dual-alloyed into n-type Pnma-phase SnS crystals to achieve a considerable boost in carrier concentration, and the resultant triple-conduction-band activation significantly decouples carrier mobility and effective mass, facilitating a substantial enhancement in the out-of-plane three-dimensional (3D) charge transport. Meanwhile, the 2D phonon transport is further strengthened by the reduced group velocities and low-lying optical phonon modes, significantly suppressing the lattice thermal conductivity. Consequently, an exceptional out-of-plane ZT exceeding 2.0 at 698 K and an average ZT higher than 1.1 at 300–723 K are achieved in n-type Sn0.63Pb0.37S0.55Se0.45crystals within the Pnma-phase region. Furthermore, the as-fabricated single-leg thermoelectric device demonstrates a power generation efficiency of ∼8.3% under a temperature difference (ΔT) of 472 K, showing promise for n-type thermoelectric sulfides. This work marks a significant advancement in the earth-abundant n-type SnS thermoelectrics through triple-conduction-band engineering, promoting the construction and potential application of all SnS-based devices.
AB - The increasing interest for high-performance and earth-abundant thermoelectrics has motivated attention toward sulfide-based compounds. Among them, tin sulfide (SnS) has emerged as a promising candidate, especially in its p-type form. However, progress in n-type SnS has been hindered by poor electrical transport. In this study, Se and Pb are dual-alloyed into n-type Pnma-phase SnS crystals to achieve a considerable boost in carrier concentration, and the resultant triple-conduction-band activation significantly decouples carrier mobility and effective mass, facilitating a substantial enhancement in the out-of-plane three-dimensional (3D) charge transport. Meanwhile, the 2D phonon transport is further strengthened by the reduced group velocities and low-lying optical phonon modes, significantly suppressing the lattice thermal conductivity. Consequently, an exceptional out-of-plane ZT exceeding 2.0 at 698 K and an average ZT higher than 1.1 at 300–723 K are achieved in n-type Sn0.63Pb0.37S0.55Se0.45crystals within the Pnma-phase region. Furthermore, the as-fabricated single-leg thermoelectric device demonstrates a power generation efficiency of ∼8.3% under a temperature difference (ΔT) of 472 K, showing promise for n-type thermoelectric sulfides. This work marks a significant advancement in the earth-abundant n-type SnS thermoelectrics through triple-conduction-band engineering, promoting the construction and potential application of all SnS-based devices.
UR - https://www.scopus.com/pages/publications/105023713801
U2 - 10.1021/jacs.5c18076
DO - 10.1021/jacs.5c18076
M3 - 文章
C2 - 41258676
AN - SCOPUS:105023713801
SN - 0002-7863
VL - 147
SP - 44572
EP - 44580
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
IS - 48
ER -