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

Journal Article · · Angewandte Chemie
 [1];  [2];  [3];  [1];  [2];  [4];  [5];  [6];  [7];  [2];  [6];  [6]
  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

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 GeAg0.2Sb0.2Se1.4 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.

Research Organization:
Energy Frontier Research Centers (EFRC) (United States). Solid-State Solar-Thermal Energy Conversion Center (S3TEC)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Natural Science Foundation of China (NNSF)
Grant/Contract Number:
SC0001299; FG02-09ER46577
OSTI ID:
1470454
Journal Information:
Angewandte Chemie, Vol. 129, Issue 45; Related Information: S3TEC partners with Massachusetts Institute of Technology (lead); Boston College; Oak Ridge National Laboratory; Rensselaer Polytechnic Institute; ISSN 0044-8249
Publisher:
German Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English

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Temperature Dependent n-Type Self Doping in Nominally 19-Electron Half-Heusler Thermoelectric Materials journal September 2018
Stabilizing n‐Type Cubic GeSe by Entropy‐Driven Alloying of AgBiSe 2 : Ultralow Thermal Conductivity and Promising Thermoelectric Performance journal October 2018
Cation-Tuned Synthesis of Fluorooxoborates: Towards Optimal Deep-Ultraviolet Nonlinear Optical Materials journal January 2018
Soft Phonon Modes Leading to Ultralow Thermal Conductivity and High Thermoelectric Performance in AgCuTe journal March 2018
Stabilizing n‐Type Cubic GeSe by Entropy‐Driven Alloying of AgBiSe 2 : Ultralow Thermal Conductivity and Promising Thermoelectric Performance journal November 2018
Cation-Tuned Synthesis of Fluorooxoborates: Towards Optimal Deep-Ultraviolet Nonlinear Optical Materials journal January 2018
Texture Development and Grain Alignment of Hot‐Pressed Tetradymite Bi 0.48 Sb 1.52 Te 3 via Powder Molding journal September 2019
Unraveling a novel ferroelectric GeSe phase and its transformation into a topological crystalline insulator under high pressure journal September 2018
Significantly optimized thermoelectric properties in high-symmetry cubic Cu 7 PSe 6 compounds via entropy engineering journal January 2018
Synergetic optimization of electronic and thermal transport for high-performance thermoelectric GeSe–AgSbTe 2 alloy journal January 2018
First-principles prediction of the native filament:dielectric interfaces for the possible filamentary switching mechanism in chalcogenide selector devices journal January 2020
Recent advances in non-Pb-based group-IV chalcogenides for environmentally-friendly thermoelectric materials journal April 2018
Soft Phonon Modes Leading to Ultralow Thermal Conductivity and High Thermoelectric Performance in AgCuTe journal March 2018