期刊
JOURNAL OF ADVANCED CERAMICS
卷 12, 期 3, 页码 539-552出版社
TSINGHUA UNIV PRESS
DOI: 10.26599/JAC.2023.9220702
关键词
p-type skutterudite materials; Ni doping; synergistic optimization; thermoelectric (TE) properties
By doping Ni in the Fe sites of p-type CeFe3.8Co0.2Sb12 skutterudite, impurity phases with high thermal conductivity can be reduced and carrier concentration can be regulated, leading to a significant increase in the Seebeck coefficient. The thermal conductivity is suppressed due to enhanced point defect phonon scattering and decreased hole concentration. The introduction of Ni doping results in a TE figure of merit ZT of 0.8, approximately 50% higher than that of a Ni-free sample. Thus, this study provides a strategy to synergistically optimize the electrical-thermal performances of skutterudites by alloying engineering.
The enhancements in thermoelectric (TE) performances of p-type skutterudites are usually limited due to the relatively low Seebeck coefficients owing to the higher carrier concentration and more impurity phases induced by inherent structural instability of a Fe-based skutterudite. As shown in this study, alloying engineering of Ni doping at Fe sites in a p-type CeFe3.8Co0.2Sb12 skutterudite can not only reduce the impurity phases with high thermal conductivity but also regulate the carrier concentration, and thus significantly increase the Seebeck coefficient. The thermal conductivity was largely suppressed due to the enhanced point defect phonon scattering and decreased hole concentration. As a result, a TE figure of merit ZT of the CeFe3.5Ni0.3Co0.2Sb12 sample reached 0.8, which is approximately 50% higher than that of a Ni-free sample. Appropriate Ni doping can maintain a high ZT at a high temperature by controlling the reduction in a band gap. Therefore, a high average ZT close to 0.8 at 650-800 K for CeFe3.5Ni0.3Co0.2Sb12 was obtained, which was comparable to or even higher than those of the reported Ce-filled Fe-based skutterudites due to the synergistic optimization of electrical and thermal performances. This study provides a strategy to synergistically optimize electrical-thermal performances of the p-type skutterudites by alloying engineering.
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