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

Hu，Lei1,2; Luo，Yubo1,2; Fang，Yue Wen3; Qin，Feiyu3; Cao，Xun1; Xie，Hongyao2; Liu，Jiawei1; Dong，Jinfeng1; Sanson，Andrea4; Giarola，Marco5; Tan，Xianyi1,6; Zheng，Yun1; Suwardi，Ady6; Huang，Yizhong1; Hippalgaonkar，Kedar1,6; He，Jiaqing7; Zhang，Wenqing7; Xu，Jianwei6; Yan，Qingyu1; Kanatzidis，Mercouri G.2

2021

10.1002/aenm.202100661

Advanced Energy Materials   影响因子和分区

1614-6832

1614-6840

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, it is reported that the triple doping of CuSnSe leads to a high ZT value of 1.6 at 823 K for CuAg(SnGaNa)Se, and a decent average ZT (ZT) value of 0.7 is also achieved for CuAg(SnMgNa)Se from 475 to 823 K. This 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 CuSnSe into a cubic structure. This symmetry enhancing leads to an increase in the effective mass from 0.8 m to 2.6 m (m, free electron mass) and the power factor from 4.3 µW cm K for CuSnSe to 11.6 µW cm K. 3) Na doping creates dense dislocation arrays and nanoprecipitates, which strengthens the phonon scattering. 4) Pair distribution function analysis shows localized symmetry breakdown in the cubic CuAg(SnGaNa)Se. This work provides a standpoint to design promising thermoelectric materials by synergistically manipulating crystal symmetry and nanoscale defects.

crystal symmetry diamondoid structure nanoscale defects thermoelectrics

SCI ; EI

英语

其他

WOS:000705536900001

20214111001802

Crystal symmetry ; Distribution functions ; Eigenvalues and eigenfunctions ; Electronic structure ; Electrons ; Nanostructured materials ; Phonons ; Point defects ; Precipitation (chemical) ; Silver compounds ; Sodium compounds ; Thermal conductivity ; Thermoelectric equipment ; Thermoelectricity ; Tin compounds

Thermoelectric Energy:615.4 ; Thermodynamics:641.1 ; Electricity: Basic Concepts and Phenomena:701.1 ; Nanotechnology:761 ; Chemical Operations:802.3 ; Probability Theory:922.1 ; Crystalline Solids:933.1 ; Crystal Lattice:933.1.1

2-s2.0-85116574615

Scopus

1.School of Materials Science and Engineering,Nanyang Technological University,Singapore,639798,Singapore
2.Department of Chemistry,Northwestern University,Evanston,60208,United States
3.Materials and Structure Laboratory,Tokyo Institute of Technology,Yokohama,226-8503,Japan
4.Department of Physics and Astronomy,University of Padova,Padova,I-35131,Italy
5.Department of Computer Science,University of Verona,Italy University of Verona,Verona,Ca’ Vignal 2, Strada le Grazie 15,I-37134,Italy
6.Institute of Materials Research and Engineering,A*STAR Agency for Science,Technology and Research,Singapore,138634,Singapore
7.Department of Physics,Southern University of Science and Technology,Shenzhen,518055,China

Hu，Lei,Luo，Yubo,Fang，Yue Wen,et al. High Thermoelectric Performance through Crystal Symmetry Enhancement in Triply Doped Diamondoid Compound Cu2SnSe3[J]. Advanced Energy Materials,2021,11.

Hu，Lei.,Luo，Yubo.,Fang，Yue Wen.,Qin，Feiyu.,Cao，Xun.,...&Kanatzidis，Mercouri G..(2021).High Thermoelectric Performance through Crystal Symmetry Enhancement in Triply Doped Diamondoid Compound Cu2SnSe3.Advanced Energy Materials,11.

Hu，Lei,et al."High Thermoelectric Performance through Crystal Symmetry Enhancement in Triply Doped Diamondoid Compound Cu2SnSe3".Advanced Energy Materials 11(2021).