期刊
SCIENCE AND TECHNOLOGY OF ADVANCED MATERIALS
卷 22, 期 1, 页码 363-372出版社
TAYLOR & FRANCIS LTD
DOI: 10.1080/14686996.2021.1920821
关键词
Co-doped Cu2SnS3; sb-substitution; carrier compensation; polymorphic; thermoelectric
资金
- National Natural Science Foundation of China [51672127]
- China Key National PD Plan [2017YFA0700705]
- Priority Academic Program Development of Jiangsu Higher Education Institutions
By doping Sb at the Sn site in Cu2Sn0.8Co0.2S3, the Seebeck coefficient can be effectively enhanced, the electronic thermal conductivity reduced, and a peak ZT of approximately 0.88 at 773 K achieved.
Heavily acceptor-doped Cu2SnS3 (CTS) shows promisingly large power factor (PF) due to its rather high electrical conductivity (sigma) which causes a modest ZT with a high electronic thermal conductivity (k(e)). In the present work, a strategy of carrier compensation through Sb-doping at the Sn site in Cu2Sn0.8Co0.2S3 was investigated, aiming at tailoring electrical and phonon transport properties simultaneously. Rietveld analysis suggested a complex polymorphic microstructure in which the cation-(semi)ordered tetragonal phase becomes dominant over the coherently bonded cation-disordered cubic phase, as is preliminarily revealed using TEM observation, upon Sb-doping and Sb would substitute Sn preferentially in the tetragonal structure. With increasing content of Sb, the s was lowered and the Seebeck coefficient (S) was enhanced effectively, which gave rise to high PFs maintained at similar to 10.4 mu Wcm(-1)K(-2) at 773 K together with an optimal reduction in Kappa(e) by 60-70% in the whole temperature range. The lattice thermal conductivity was effectively suppressed from 1.75 Wm(-1)K(-1) to similar to 1.2 Wm(-1)K(-1) at 323 K while maintained very low at 0.3-0.4 Wm(-1)K(-1) at 773 K. As a result, a peak ZT of similar to 0.88 at 773 K has been achieved for Cu(2)Sn(0.7)4Sb(0.06)Co(0.2)S(3), which stands among the tops so far of the CTS-based diamond-like ternary sulfides. These findings demonstrate that polymorphic microstructures with cation-disordered interfaces as an approach to achieve effective phonon-blocking and low lattice thermal conductivity, of which further crystal chemistry, microstructural and electrical tailoring are possible by appropriate doping. [GRAPHICS]
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