The Role of Zn in Chalcopyrite CuFeS2: Enhanced Thermoelectric Properties of Cu1–xZnxFeS2 with In Situ Nanoprecipitates
Abstract
Chalcopyrite (CuFeS2) is a widespread natural mineral, composed of earth–abundant and nontoxic elements. It has been considered a promising n–type material for thermoelectric applications. In this work, a series of Zn–doped Cu1–xZnxFeS2 (x = 0–0.1) compounds are synthesized by vacuum melting combined with the plasma activated sintering process. The role of Zn in the chalcopyrite and its different effects on thermoelectric properties, depending on its concentration and location in the crystal lattice, are discussed. It is found that Zn is an effective donor which increases the carrier concentration and improves the thermoelectric properties of CuFeS2. Here, when the content of Zn exceeds the solubility limit, Zn partially enters the Cu sites and forms in situ ZnS nanophase. This, in turn, shifts the balance between the anion and cation species which is re–established by the formation of antisite Fe/Cu defects. Beyond maintaining charge neutrality of the structure, such antisite defects relieve the lattice strain in the matrix and increase the solubility of Zn further. The highest ZT value of 0.26 is achieved at 630 K for Cu0.92Zn0.08FeS2, which represents an enhancement of about 80% over that of the pristine CuFeS2 sample.
- Authors:
-
- Wuhan University of Technology (China)
- University of Michigan, Ann Arbor, MI (United States)
- Northwestern University, Evanston, IL (United States)
- Publication Date:
- Research Org.:
- Univ. of Michigan, Ann Arbor, MI (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); Natural Science Foundation of China
- OSTI Identifier:
- 1533065
- Alternate Identifier(s):
- OSTI ID: 1401491
- Grant/Contract Number:
- PI0000012; 51402222; 51172174; 51521001; 51632006; SC000105
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Advanced Energy Materials
- Additional Journal Information:
- Journal Volume: 7; Journal Issue: 3; Journal ID: ISSN 1614-6832
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; Chemistry; Energy & Fuels; Materials Science; Physics; Environmentally friendly; In situ Nanoprecipitates; Thermal resistance; Thermoelectric
Citation Formats
Xie, Hongyao, Su, Xianli, Zheng, Gang, Zhu, Ting, Yin, Kang, Yan, Yonggao, Uher, Ctirad, Kanatzidis, Mercouri G., and Tang, Xinfeng. The Role of Zn in Chalcopyrite CuFeS2: Enhanced Thermoelectric Properties of Cu1–xZnxFeS2 with In Situ Nanoprecipitates. United States: N. p., 2016.
Web. doi:10.1002/aenm.201601299.
Xie, Hongyao, Su, Xianli, Zheng, Gang, Zhu, Ting, Yin, Kang, Yan, Yonggao, Uher, Ctirad, Kanatzidis, Mercouri G., & Tang, Xinfeng. The Role of Zn in Chalcopyrite CuFeS2: Enhanced Thermoelectric Properties of Cu1–xZnxFeS2 with In Situ Nanoprecipitates. United States. https://doi.org/10.1002/aenm.201601299
Xie, Hongyao, Su, Xianli, Zheng, Gang, Zhu, Ting, Yin, Kang, Yan, Yonggao, Uher, Ctirad, Kanatzidis, Mercouri G., and Tang, Xinfeng. Thu .
"The Role of Zn in Chalcopyrite CuFeS2: Enhanced Thermoelectric Properties of Cu1–xZnxFeS2 with In Situ Nanoprecipitates". United States. https://doi.org/10.1002/aenm.201601299. https://www.osti.gov/servlets/purl/1533065.
@article{osti_1533065,
title = {The Role of Zn in Chalcopyrite CuFeS2: Enhanced Thermoelectric Properties of Cu1–xZnxFeS2 with In Situ Nanoprecipitates},
author = {Xie, Hongyao and Su, Xianli and Zheng, Gang and Zhu, Ting and Yin, Kang and Yan, Yonggao and Uher, Ctirad and Kanatzidis, Mercouri G. and Tang, Xinfeng},
abstractNote = {Chalcopyrite (CuFeS2) is a widespread natural mineral, composed of earth–abundant and nontoxic elements. It has been considered a promising n–type material for thermoelectric applications. In this work, a series of Zn–doped Cu1–xZnxFeS2 (x = 0–0.1) compounds are synthesized by vacuum melting combined with the plasma activated sintering process. The role of Zn in the chalcopyrite and its different effects on thermoelectric properties, depending on its concentration and location in the crystal lattice, are discussed. It is found that Zn is an effective donor which increases the carrier concentration and improves the thermoelectric properties of CuFeS2. Here, when the content of Zn exceeds the solubility limit, Zn partially enters the Cu sites and forms in situ ZnS nanophase. This, in turn, shifts the balance between the anion and cation species which is re–established by the formation of antisite Fe/Cu defects. Beyond maintaining charge neutrality of the structure, such antisite defects relieve the lattice strain in the matrix and increase the solubility of Zn further. The highest ZT value of 0.26 is achieved at 630 K for Cu0.92Zn0.08FeS2, which represents an enhancement of about 80% over that of the pristine CuFeS2 sample.},
doi = {10.1002/aenm.201601299},
journal = {Advanced Energy Materials},
number = 3,
volume = 7,
place = {United States},
year = {Thu Oct 27 00:00:00 EDT 2016},
month = {Thu Oct 27 00:00:00 EDT 2016}
}
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