High thermoelectric performance through crystal symmetry enhancement in triply doped diamondoid compound Cu₂SnSe₃
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, n...
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Engineering::Materials Crystal Symmetry Diamondoid Structure Hu, Lei Luo, Yubo Fang, Yue-Wen Qin, Feiyu Cao, Xun Xie, Hongyao Liu, Jiawei Dong, Jinfeng Sanson, Andrea Giarola, Marco Tan, Xian Yi Zheng, Yun Suwardi, Ady Huang, Yizhong Hippalgaonkar, Kedar He, Jiaqing Zhang, Wenqing Xu, Jianwei Yan, Qingyu Kanatzidis, Mercouri G. High thermoelectric performance through crystal symmetry enhancement in triply doped diamondoid compound Cu₂SnSe₃ |
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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 Cu2SnSe3 leads to a high ZT value of 1.6 at 823 K for Cu1.85Ag0.15(Sn0.88Ga0.1Na0.02)Se3, and a decent average ZT (ZTave) value of 0.7 is also achieved for Cu1.85Ag0.15(Sn0.93Mg0.06Na0.01)Se3 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 Cu2SnSe3 into a cubic structure. This symmetry enhancing leads to an increase in the effective mass from 0.8 me to 2.6 me (me, free electron mass) and the power factor from 4.3 µW cm−1 K−2 for Cu2SnSe3 to 11.6 µW cm−1 K−2. 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 Cu1.85Ag0.15(Sn0.88Ga0.1Na0.02)Se3. This work provides a standpoint to design promising thermoelectric materials by synergistically manipulating crystal symmetry and nanoscale defects. |
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School of Materials Science and Engineering |
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School of Materials Science and Engineering Hu, Lei Luo, Yubo Fang, Yue-Wen Qin, Feiyu Cao, Xun Xie, Hongyao Liu, Jiawei Dong, Jinfeng Sanson, Andrea Giarola, Marco Tan, Xian Yi Zheng, Yun Suwardi, Ady Huang, Yizhong Hippalgaonkar, Kedar He, Jiaqing Zhang, Wenqing Xu, Jianwei Yan, Qingyu Kanatzidis, Mercouri G. |
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Article |
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Hu, Lei Luo, Yubo Fang, Yue-Wen Qin, Feiyu Cao, Xun Xie, Hongyao Liu, Jiawei Dong, Jinfeng Sanson, Andrea Giarola, Marco Tan, Xian Yi Zheng, Yun Suwardi, Ady Huang, Yizhong Hippalgaonkar, Kedar He, Jiaqing Zhang, Wenqing Xu, Jianwei Yan, Qingyu Kanatzidis, Mercouri G. |
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Hu, Lei |
title |
High thermoelectric performance through crystal symmetry enhancement in triply doped diamondoid compound Cu₂SnSe₃ |
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High thermoelectric performance through crystal symmetry enhancement in triply doped diamondoid compound Cu₂SnSe₃ |
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High thermoelectric performance through crystal symmetry enhancement in triply doped diamondoid compound Cu₂SnSe₃ |
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High thermoelectric performance through crystal symmetry enhancement in triply doped diamondoid compound Cu₂SnSe₃ |
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High thermoelectric performance through crystal symmetry enhancement in triply doped diamondoid compound Cu₂SnSe₃ |
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high thermoelectric performance through crystal symmetry enhancement in triply doped diamondoid compound cu₂snse₃ |
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2022 |
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https://hdl.handle.net/10356/159231 |
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sg-ntu-dr.10356-1592312023-07-14T16:05:33Z 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, Xian Yi Zheng, Yun Suwardi, Ady Huang, Yizhong Hippalgaonkar, Kedar He, Jiaqing Zhang, Wenqing Xu, Jianwei Yan, Qingyu Kanatzidis, Mercouri G. School of Materials Science and Engineering Institute of Materials Research and Engineering, A*STAR Engineering::Materials Crystal Symmetry Diamondoid Structure 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 Cu2SnSe3 leads to a high ZT value of 1.6 at 823 K for Cu1.85Ag0.15(Sn0.88Ga0.1Na0.02)Se3, and a decent average ZT (ZTave) value of 0.7 is also achieved for Cu1.85Ag0.15(Sn0.93Mg0.06Na0.01)Se3 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 Cu2SnSe3 into a cubic structure. This symmetry enhancing leads to an increase in the effective mass from 0.8 me to 2.6 me (me, free electron mass) and the power factor from 4.3 µW cm−1 K−2 for Cu2SnSe3 to 11.6 µW cm−1 K−2. 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 Cu1.85Ag0.15(Sn0.88Ga0.1Na0.02)Se3. This work provides a standpoint to design promising thermoelectric materials by synergistically manipulating crystal symmetry and nanoscale defects. Agency for Science, Technology and Research (A*STAR) Ministry of Education (MOE) Submitted/Accepted version This work was supported by the U.S. Department of Energy, Office of Science Basic Energy Sciences under grant DE-SC0014520, DOE Office of Science (materials characterization, sample synthesis, transport properties). User Facilities were supported by the Office of Science of the U.S. Department of Energy under Contract Nos. DE-AC02-06CH11357 and DE-AC02-05CH11231. Access to facilities of high-performance computational resources at the Northwestern University is acknowledged. The authors also acknowledge Singapore MOE Tier 2 under Grant Nos. MOE2018-T2-1-010, Singapore A*STAR Pharos Program SERC 1527200022, and Singapore A*STAR project A19D9a0096. 2022-06-01T07:19:46Z 2022-06-01T07:19:46Z 2021 Journal Article Hu, L., Luo, Y., Fang, Y., Qin, F., Cao, X., Xie, H., Liu, J., Dong, J., Sanson, A., Giarola, M., Tan, X. Y., Zheng, Y., Suwardi, A., Huang, Y., Hippalgaonkar, K., He, J., Zhang, W., Xu, J., Yan, Q. & Kanatzidis, M. G. (2021). High thermoelectric performance through crystal symmetry enhancement in triply doped diamondoid compound Cu₂SnSe₃. Advanced Energy Materials, 11(42), 2100661-. https://dx.doi.org/10.1002/aenm.202100661 1614-6832 https://hdl.handle.net/10356/159231 10.1002/aenm.202100661 2-s2.0-85116574615 42 11 2100661 en MOE2018-T2-1-010 SERC 1527200022 A19D9a0096 Advanced Energy Materials This is the peer reviewed version of the following article: Hu, L., Luo, Y., Fang, Y., Qin, F., Cao, X., Xie, H., Liu, J., Dong, J., Sanson, A., Giarola, M., Tan, X. Y., Zheng, Y., Suwardi, A., Huang, Y., Hippalgaonkar, K., He, J., Zhang, W., Xu, J., Yan, Q. & Kanatzidis, M. G. (2021). High thermoelectric performance through crystal symmetry enhancement in triply doped diamondoid compound Cu₂SnSe₃. Advanced Energy Materials, 11(42), 2100661-, which has been published in final form at https://doi.org/10.1002/aenm.202100661. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Use of Self-Archived Versions. application/pdf |