TY - JOUR
T1 - Robustly Boosting Thermoelectric Performance of N-Type PbSe via Lattice Plainification and Dynamic Doping
AU - Gao, Dezheng
AU - Wen, Yi
AU - Bai, Shulin
AU - Wang, Siqi
AU - Liu, Shibo
AU - Li, Yichen
AU - Wang, Lei
AU - Zang, Wujing
AU - Su, Xianli
AU - Gao, Xiang
AU - Xie, Hongyao
AU - Zhao, Li Dong
N1 - Publisher Copyright:
© 2024 Wiley-VCH GmbH.
PY - 2024/12/12
Y1 - 2024/12/12
N2 - Ideal thermoelectrics shall possess a high average ZT, which relies on high carrier mobility and appropriate carrier density at operating temperature. However, conventional doping usually results in a temperature-independent carrier concentration, making performance optimization over a wide temperature range be challenging. This work demonstrates the combination of lattice plainification and dynamic doping strategies is an effective route to boost the average ZT of N-type PbSe. Because Sn and Pb have similar ionic radii and electronegativity, this allows Sn to fill the intrinsic Pb vacancies and effectively improves the carrier mobility of PbSe to 1300 cm2 V−1 s−1. Furthermore, a trace amount of Cu is introduced into the Sn-filled PbSe to optimize the carrier concentration. The extra Cu is situated in the interstitial sides of the lattice, which undergoes a dissolution-precipitation process with temperature, leading to a strongly temperature-dependent carrier density in the material. This dynamic doping effectively improves the electrical transport properties and is also valid to suppress the lattice thermal conductivity. Ultimately, the resulting PbSn0.004Se+3‰Cu obtains a maximum ZT of ≈1.7 at 800 K and an average ZT of ≈1.0, with a 7.7% power generation efficiency in a single-arm device, showing significant potential for commercial application.
AB - Ideal thermoelectrics shall possess a high average ZT, which relies on high carrier mobility and appropriate carrier density at operating temperature. However, conventional doping usually results in a temperature-independent carrier concentration, making performance optimization over a wide temperature range be challenging. This work demonstrates the combination of lattice plainification and dynamic doping strategies is an effective route to boost the average ZT of N-type PbSe. Because Sn and Pb have similar ionic radii and electronegativity, this allows Sn to fill the intrinsic Pb vacancies and effectively improves the carrier mobility of PbSe to 1300 cm2 V−1 s−1. Furthermore, a trace amount of Cu is introduced into the Sn-filled PbSe to optimize the carrier concentration. The extra Cu is situated in the interstitial sides of the lattice, which undergoes a dissolution-precipitation process with temperature, leading to a strongly temperature-dependent carrier density in the material. This dynamic doping effectively improves the electrical transport properties and is also valid to suppress the lattice thermal conductivity. Ultimately, the resulting PbSn0.004Se+3‰Cu obtains a maximum ZT of ≈1.7 at 800 K and an average ZT of ≈1.0, with a 7.7% power generation efficiency in a single-arm device, showing significant potential for commercial application.
KW - PbSe
KW - dissolution–precipitation
KW - dynamic doping
KW - lattice plainification
UR - https://www.scopus.com/pages/publications/85205215103
U2 - 10.1002/smll.202407556
DO - 10.1002/smll.202407556
M3 - 文章
C2 - 39344539
AN - SCOPUS:85205215103
SN - 1613-6810
VL - 20
JO - Small
JF - Small
IS - 50
M1 - 2407556
ER -