All-Scale Hierarchically Structured p-Type PbSe Alloys with High Thermoelectric Performance Enabled by Improved Band Degeneracy

Tan, Gangjian; Hao, Shiqiang; Cai, Songting; Bailey, Trevor P.; Luo, Zhongzhen; Hadar, Ido; Uher, Ctirad; Dravid, Vinayak P.; Wolverton, Christopher; Kanatzidis, Mercouri G.

doi:10.1021/jacs.9b00967

Title: All-Scale Hierarchically Structured p-Type PbSe Alloys with High Thermoelectric Performance Enabled by Improved Band Degeneracy

Journal Article · Tue Feb 19 00:00:00 EST 2019 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.9b00967· OSTI ID:1777264

^[1]; Hao, Shiqiang ^[2]; Cai, Songting ^[2]; Bailey, Trevor P. ^[3]; Luo, Zhongzhen ^[2];

^[2]; Uher, Ctirad ^[3];

^[2];

^[2]

Wuhan Univ. of Technology (China)
Northwestern Univ., Evanston, IL (United States)
Univ. of Michigan, Ann Arbor, MI (United States)

We show an example of hierarchically designing electronic bands of PbSe toward excellent thermoelectric performance. We find that alloying 15 mol % PbTe into PbSe causes a negligible change in the light and heavy valence band energy offsets (ΔE_V) of PbSe around room temperature; however, with rising temperature it makes ΔE_V decrease at a significantly higher rate than in PbSe. In other words, the temperature-induced valence band convergence of PbSe is accelerated by alloying with PbTe. On this basis, applying 3 mol % Cd substitution on the Pb sites of PbSe_0.85Te_0.15 decreases ΔE_V and enhances the Seebeck coefficient at all temperatures. Here, excess Cd precipitates out as CdSe_1-yTe_y, whose valence band aligns with that of the p-type Na-doped PbSe_0.85Te_0.15 matrix. This enables facile charge transport across the matrix/precipitate interfaces and retains the high carrier mobilities. Meanwhile, compared to PbSe the lattice thermal conductivity of PbSe_0.85Te_0.15 is significantly decreased to its amorphous limit of 0.5 W m^-1 K^-1. Consequently, a highest peak ZT of 1.7 at 900 K and a record high average ZT of ~1 (400-900 K) for a PbSe-based system are achieved in the composition Pb_0.95Na_0.02Cd_0.03Se_0.85Te_0.15, which are ~70% and ~50% higher than those of Pb_0.98Na_0.02Se control sample, respectively.

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Research Organization:: Northwestern Univ., Evanston, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); ONR; Natural Science Foundation of China

Grant/Contract Number:: SC0014520; N00014-18-1-2102; 11804261

OSTI ID:: 1777264

Journal Information:: Journal of the American Chemical Society, Vol. 141, Issue 10; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 66 works

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Title: All-Scale Hierarchically Structured p-Type PbSe Alloys with High Thermoelectric Performance Enabled by Improved Band Degeneracy

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