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Title: Ultralow Thermal Conductivity in Diamondoid Structures and High Thermoelectric Performance in (Cu 1– x Ag x )(In 1– y Ga y )Te 2

Journal Article · · Journal of the American Chemical Society
DOI:https://doi.org/10.1021/jacs.1c01801· OSTI ID:1858071

Owing to the diversity of composition and excellent transport properties, the ternary I-III-VI2type diamond-like chalcopyrite compounds are attractive functional semiconductors including as thermoelectric materials. In this family,CuInTe2 and CuGaTe2 are well investigated and achieve maximum ZT values of ~1.4 at 950 K and an average ZT of 0.43. However, both compounds have poor electrical conductivity at low temperature, resulting in low ZT below 450K. In this work, we have greatly improved the thermoelectric performance in the quinary diamondoid compound (Cu0.8Ag0.2)(In0.2Ga0.8)Te2 by understanding and controlling the effects of different constituent elements on the thermoelectric transport properties. Our combined theoretical and experimental effort indicates that Gain the In site of the lattice decreases the density-of-states carrier effective mass and improves the electrical conductivity and power factor of Cu0.8Ag0.2In1-xGaxTe2. Furthermore, Ag in the Cu site strongly suppresses the heat transport via the enhanced acoustic phonon-optical phonon coupling effects, leading to the ultra low thermal conductivity of ~0.49 Wm-1 K-1 at 850 K in Cu0.8Ag0.2In0.2Ga0.8Te2. Defect formation energy calculations suggest intrinsic Cu vacancies introduce defect levels that are important to the temperature-dependent hole density and electrical conductivity; therefore, we introduced extra Cu vacancies to optimize the hole carrier density and improve the power factor of Cu0.8Ag0.2In0.2Ga0.8Te2. Finally, as a result, a maximum ZT of ~1.5 at 850 K and an average ZT of 0.78 in the temperature range of 400-850 K are obtained, which is among the highest in the diamond-like compound family.

Research Organization:
Northwestern Univ., Evanston, IL (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Sciences Foundation (NSF); Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource
Grant/Contract Number:
SC0014520; AC02-06CH11357; AC02-05CH11231; ECCS 2025633; DMR-1720139
OSTI ID:
1858071
Alternate ID(s):
OSTI ID: 1834039
Journal Information:
Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Vol. 143 Journal Issue: 15; ISSN 0002-7863
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English

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