Amphoteric Indium Enables Carrier Engineering to Enhance the Power Factor and Thermoelectric Performance in n-Type AgnPb100InnTe100+2n (LIST)

Xiao, Yu; Wu, Haijun; Wang, Dongyang; Niu, Changlei; Pei, Yanling; Zhang, Yang; Spanopoulos, Ioannis; Witting, Ian Thomas; Li, Xin; Pennycook, Stephen J.; Snyder, Gerald Jeffrey; Kanatzidis, Mercouri G.; Zhao, Li‐Dong

doi:10.1002/aenm.201900414

Amphoteric Indium Enables Carrier Engineering to Enhance the Power Factor and Thermoelectric Performance in n-Type Ag_nPb₁₀₀In_nTe_100+2n (LIST)

Journal Article · Thu Mar 07 04:00:00 EST 2019 · Advanced Energy Materials

DOI:https://doi.org/10.1002/aenm.201900414· OSTI ID:1777378

Xiao, Yu ^[1]; Wu, Haijun ^[2]; Wang, Dongyang ^[3]; Niu, Changlei ^[4]; Pei, Yanling ^[3]; Zhang, Yang ^[2]; Spanopoulos, Ioannis ^[5]; Witting, Ian Thomas ^[5]; Li, Xin ^[4]; Pennycook, Stephen J. ^[2]; Snyder, Gerald Jeffrey ^[5]; Kanatzidis, Mercouri G. ^[5]; ^[3]

Beihang Univ., Beijing (China); Northwestern University
National Univ. of Singapore (Singapore)
Beihang Univ., Beijing (China)
China Inst. of Atomic Energy, Beijing (China)
Northwestern Univ., Evanston, IL (United States)

The Ag and In co-doped PbTe, Ag_nPb₁₀₀In_nTe_100+2n (LIST), exhibits n-type behavior and features unique inherent electronic levels that induce self-tuning carrier density. Results show that In is amphoteric in the LIST, forming both In³⁺ and In¹⁺ centers. Through unique interplay of valence fluctuations in the In centers and conduction band filling, the electron carrier density can be increased from ≈3.1 × 10¹⁸ cm^-3 at 323 K to ≈2.4 × 10¹⁹ cm^-3 at 820 K, leading to large power factors peaking at ≈16.0 μWcm^-1 K^-2 at 873 K. The lone pair of electrons from In⁺ can be thermally continuously promoted into the conduction band forming In³⁺, consistent with the amphoteric character of In. Moreover, with rising temperature, the Fermi level shifts into the conduction band, which enlarges the optical band gap based on the Moss–Burstein effect, and reduces bipolar diffusion and thermal conductivity. Adding extra Ag in LIST improves the electrical transport properties and meanwhile lowers the lattice thermal conductivity to ≈0.40 Wm^-1 K^-1. Here, the addition of Ag creates spindle-shaped Ag₂Te nanoprecipitates and atomic-scale interstitials that scatter a broader set of phonons. As a result, a maximum ZT value ≈1.5 at 873 K is achieved in Ag₆Pb₁₀₀InTe₁₀₂ (LIST).

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Key Research and Development Program of China; National Natural Science Foundation of China; NSF

Grant/Contract Number:: SC0014520

OSTI ID:: 1777378

Alternate ID(s):: OSTI ID: 1612213
OSTI ID: 1498571

Journal Information:: Advanced Energy Materials, Journal Name: Advanced Energy Materials Journal Issue: 17 Vol. 9; ISSN 1614-6832

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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LIST
ZT
bipolar diffusion
power factor
thermoelectrics