Title: High Thermoelectric Performance of New Rhombohedral Phase of GeSe stabilized through Alloying with AgSbSe₂

Abstract

GeSe is a IV–VI semiconductor, like the excellent thermoelectric materials PbTe and SnSe. Orthorhombic GeSe has been predicted theoretically to have good thermoelectric performance but is difficult to dope experimentally. Like PbTe, rhombohedral GeTe has a multivalley band structure, which is ideal for thermoelectrics and also promotes the formation of Ge vacancies to provide enough carriers for electrical transport. Herein, we investigate the thermoelectric properties of GeSe alloyed with AgSbSe₂, which stabilizes a new rhombohedral structure with higher symmetry that leads to a multivalley Fermi surface and a dramatic increase in carrier concentration. The zT of GeAg_0.2Sb_0.2Se_1.4 reaches 0.86 at 710 K, which is 18 times higher than that of pristine GeSe and over four times higher than doped orthorhombic GeSe. Our results open a new avenue towards developing novel thermoelectric materials through crystal phase engineering using a strategy of entropy stabilization of high-symmetry alloys.

Authors:

Huang, Zhiwei ^[1]; Miller, Samuel A. ^[2]; Ge, Binghui ^[3]; Yan, Mingtao ^[1]; Anand, Shashwat ^[2]; Wu, Tianmin ^[4]; Nan, Pengfei ^[5]; Zhu, Yuanhu ^[6]; Zhuang, Wei ^[7]; Snyder, G. Jeffrey ^[2]; Jiang, Peng ^[6]; Bao, Xinhe ^[6]

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+ Show Author Affiliations

1. Chinese Academy of Sciences (CAS), Dalian, Liaoning (China). CAS Center for Excellence in Nanoscience Inst. Dalian Inst. of Chemical Physics; Univ. of Chinese Academy of Sciences, Beijing (China)
2. Northwestern Univ., Evanston, IL (United States). Materials Science and Engineering Dept.
3. Chinese Academy of Sciences (CAS), Beijing (China). Beijing National Lab. for Condensed Matter Physics, Inst. of Physics
4. Chinese Academy of Sciences (CAS), Fuzhou, Fujian (China). State Key Lab. of Structural Chemistry Fujian Inst. of Research on the Structure of Matter
5. Beijing Inst. of Technology, Beijing (China). School of Physics
6. Chinese Academy of Sciences (CAS), Dalian, Liaoning (China). CAS Center for Excellence in Nanoscience Inst. Dalian Inst. of Chemical Physics
7. Chinese Academy of Sciences (CAS), Fuzhou, Fujian (China). State Key Lab. of Structural Chemistry Fujian Inst. of Research on the Structure of Matter

Publication Date:

2017-09-20

Research Org.:

Energy Frontier Research Centers (EFRC) (United States). Solid-State Solar-Thermal Energy Conversion Center (S3TEC)

Sponsoring Org.:

USDOE Office of Science (SC), Basic Energy Sciences (BES); National Natural Science Foundation of China (NNSF)

OSTI Identifier:

1470454

Grant/Contract Number:  

SC0001299; FG02-09ER46577

Resource Type:

Accepted Manuscript

Journal Name:

Angewandte Chemie

Additional Journal Information:

Journal Volume: 129; Journal Issue: 45; Related Information: S3TEC partners with Massachusetts Institute of Technology (lead); Boston College; Oak Ridge National Laboratory; Rensselaer Polytechnic Institute; Journal ID: ISSN 0044-8249

Publisher:

German Chemical Society

Country of Publication:

United States

Language:

English

Subject:

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; 42 ENGINEERING; 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; solar (photovoltaic); solar (thermal); solid state lighting; phonons; thermal conductivity; thermoelectric; defects; mechanical behavior; charge transport; spin dynamics; materials and chemistry by design; optics; synthesis (novel materials); synthesis (self-assembly); synthesis (scalable processing); Codotierung; Energieumwandlung; GeSe; Hochentropische Legierungen; Thermoelektrik; Co-doping; Energy conversion; Highly entropic alloys; thermoelectrics