High Thermoelectric Performance through Crystal Symmetry Enhancement in Triply Doped Diamondoid Compound Cu2SnSe3

Hu, Lei; Luo, Yubo; Fang, Yue‐Wen; Qin, Feiyu; Cao, Xun; Xie, Hongyao; Liu, Jiawei; Dong, Jinfeng; Sanson, Andrea; Giarola, Marco; Tan, Xianyi; Zheng, Yun; Suwardi, Ady; Huang, Yizhong; Hippalgaonkar, Kedar; He, Jiaqing; Zhang, Wenqing; Xu, Jianwei; Yan, Qingyu; Kanatzidis, Mercouri G.

doi:10.1002/aenm.202100661

High Thermoelectric Performance through Crystal Symmetry Enhancement in Triply Doped Diamondoid Compound Cu₂SnSe₃

Journal Article · Sat Oct 09 00:00:00 UTC 2021 · Advanced Energy Materials

DOI:https://doi.org/10.1002/aenm.202100661· OSTI ID:1834050

^[1]; ^[2]; ^[3]; ^[3]; Cao, Xun ^[4]; ^[5]; Liu, Jiawei ^[4]; Dong, Jinfeng ^[4]; ^[6]; Giarola, Marco ^[7]; ^[8]; ^[4]; ^[9]; ^[4]; ^[8]; ^[10]; ^[10]; ^[9]; ^[4]; ^[5]

Nanyang Technological Univ. (Singapore); Northwestern Univ., Evanston, IL (United States); Northwestern University
Nanyang Technological Univ. (Singapore); Northwestern Univ., Evanston, IL (United States)
Tokyo Inst. of Technology, Yokohama (Japan)
Nanyang Technological Univ. (Singapore)
Northwestern Univ., Evanston, IL (United States)
Univ. of Padova (Italy)
Univ. of Verona (Italy)
Nanyang Technological Univ. (Singapore); A*STAR Agency for Science Technology and Research (Singapore)
A*STAR Agency for Science Technology and Research (Singapore)
Southern Univ. of Science and Technology, Shenzhen (China)

The presence of high crystallographic symmetry and nanoscale defects are favorable for thermoelectrics. With proper electronic structures, a highly symmetric crystal tends to possess multiple carrier channels and promote electrical conductivity without sacrificing Seebeck coefficient. In addition, nanoscale defects can effectively scatter acoustic phonons to suppress thermal conductivity. Here, we report that the triple doping of Cu₂SnSe₃ leads to a high ZT value of 1.6 at 823 K for Cu_1.85Ag_0.15(Sn_0.88Ga_0.1Na_0.02)Se₃, and a decent average ZT (ZT_ave) value of 0.7 is also achieved for Cu_1.85Ag_0.15(Sn_0.93Mg_0.06Na_0.01)Se₃ from 475 to 823 K. Our study reveals: (1) Ag doping on Cu sites generates numerous point defects and greatly decreases lattice thermal conductivity. (2) Doping Mg or Ga converts the monoclinic Cu₂SnSe₃ into a cubic structure. This symmetry enhancing leads to increase in the effective mass from 0.8 m_e to 2.6 m_e (m_e, free electron mass) and the power factor from 4.3 μW/cm^–1K^–2 for Cu₂SnSe₃ to 11.6 μW/cm^–1K^–2. (3) Na doping creates dense dislocation arrays and nanoprecipitates, which strengthens the phonon scattering. (4) Pair distribution function analysis shows localized symmetry breakdwon in the cubic Cu_1.85Ag_0.15(Sn_0.88Ga_0.1Na_0.02)Se₃. Furthermore, the present work provides a standpoint to design promising thermoelectric materials by synergistically manipulating crystal symmetry and nanoscale defects.

View Accepted Manuscript (DOE)

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

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

Grant/Contract Number:: AC02-05CH11231; AC02-06CH11357; SC0014520

OSTI ID:: 1834050

Alternate ID(s):: OSTI ID: 1825202

Journal Information:: Advanced Energy Materials, Journal Name: Advanced Energy Materials Journal Issue: 42 Vol. 11; ISSN 1614-6832

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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High Thermoelectric Performance through Crystal Symmetry Enhancement in Triply Doped Diamondoid Compound Cu₂SnSe₃