The full-potential linear augmented plane wave method based on density functional theory is employed to investigate the electronic structure of BaSi2. With the constant relaxation time and rigid band approximation, th...The full-potential linear augmented plane wave method based on density functional theory is employed to investigate the electronic structure of BaSi2. With the constant relaxation time and rigid band approximation, the electrical conductivity, Seebeck coefficient and figure of merit are calculated by using Boltzmann transport theory, further eval- uated as a function of carrier concentration. We find that the Seebeck coefficient is more anisotropic than electrical conductivity. The figure of merit of BaSi2 is predicted to be quite high at room temperature, implying that optimal doping may be an effective way to improve thermoelectric properties.展开更多
The electronic structure and thermoelectric(TE) properties of Mg2GexSn1-x(x = 0.25, 0.50, 0.75) solid solutions are investigated by first-principles calculations and semi-classical Boltzmann theory. The special qu...The electronic structure and thermoelectric(TE) properties of Mg2GexSn1-x(x = 0.25, 0.50, 0.75) solid solutions are investigated by first-principles calculations and semi-classical Boltzmann theory. The special quasi-random structure(SQS) is used to model the solid solutions, which can produce reasonable band gaps with respect to experimental results.The n-type solid solutions have an excellent thermoelectric performance with maximum zT values exceeding 2.0, where the combination of low lattice thermal conductivity and high power factor(PF) plays an important role. These values are higher than those of pure Mg2Sn and Mg2Ge. The p-type solid solutions are inferior to the n-type ones, mainly due to the much lower PF. The maximum zT value of 0.62 is predicted for p-type Mg2Ge(0.25)Sn(0.75) at 800K. The results suggest that the n-type Mg2GexSn1-x solid solutions are promising mid-temperature TE materials.展开更多
The p-type Ge doped Fe0.4Co3.6Sb12-xGex skutterudites with multi-scaled impurity dots(500 nm-2 mm) were successfully prepared by using melt-quenching(MQ) and subsequent spark plasma sintering(SPS) technique. Com...The p-type Ge doped Fe0.4Co3.6Sb12-xGex skutterudites with multi-scaled impurity dots(500 nm-2 mm) were successfully prepared by using melt-quenching(MQ) and subsequent spark plasma sintering(SPS) technique. Compared with traditional method, the new technology significantly shortened the processing time from several days to less than 24 hours. The phase of impurity dots was demonstrated to be CoSb through analysis of X-ray diffraction(XRD) and energy-dispersive spectrum(EDS). Impurity dots were induced by Ge substitution of Sb in the non-equilibrium synthesized process. Due to the abandonment of the long reaction of annealing crystallization, a few of Ge atoms would fail to substitute Sb site of skutterudite in this non-equilibrium synthesized process, leading to that the multi-scaled impurity dots randomly distributed in the matrix of skutterudite Fe0.4Co3.6Sb12-xGex. The combination of multi-scaled impurity dots scattering long wavelength heat-carrying phonons and the point defect scattering short and middle wavelength heat-carrying phonons dramatically made the 22.2% reduction of lattice thermal conductivity. As a result, compared with unsubstituted sample of Fe0.4Co3.6Sb12, the maximum ZT value was increased by 30.5%. Thus, the two marked features of this new synthesis process, the shortened preparation time and the enhanced thermoelectric performance, would make a promising commercial application in the future.展开更多
This study prepares a group of single crystalline β-Zn_4Sb_3 with Ge and Sn codoped by the Sn-flux method according to the nominal stoichiometric ratios of Zn_(4.4)Sb_3 Ge_xSn_3(x = 0–0.15). The prepared samples...This study prepares a group of single crystalline β-Zn_4Sb_3 with Ge and Sn codoped by the Sn-flux method according to the nominal stoichiometric ratios of Zn_(4.4)Sb_3 Ge_xSn_3(x = 0–0.15). The prepared samples possess a metallic luster surface with perfect appearance and large crystal sizes. The microscopic cracks or defects are invisible in the samples from the back-scattered electron image. Except for the heavily Ge-doped sample of x = 0.15, all the samples are single phase with space group R3c. The thermal analysis results show that the samples doped with Ge exhibit an excellent thermal stability.Compared with the polycrystalline Ge-substituted β-Zn_4Sb_3, the present single crystals have higher carrier mobility, and hence the electrical conductivity is improved, which reaches 7.48×10~4S·m^(-1) at room temperature for the x = 0.1 sample.The change of Ge and Sn contents does not improve the Seebeck coefficient significantly. Benefiting from the increased electrical conductivity, the sample with x = 0.075 gets the highest power factor of 1.45×10^(-3)W·m^(-1)·K^(-2) at 543 K.展开更多
The Ba-, La- and Ag-doped polycrystalline Ca2.9M0.1Co4O9 (M=Ca, Ba, La, Ag) thermoelectric bulk samples were pre- pared via citrate acid sol-gel synthesis method followed by spark plasma sintering technique. The bul...The Ba-, La- and Ag-doped polycrystalline Ca2.9M0.1Co4O9 (M=Ca, Ba, La, Ag) thermoelectric bulk samples were pre- pared via citrate acid sol-gel synthesis method followed by spark plasma sintering technique. The bulk samples were characterized and analyzed with regard to their phase compositions, grain orientations as well as microstructures. The high temperature thermoelec- tric transport properties of the bulk samples were studied in detail. All bulk samples were found to be single-phased with modified body texture. The electrical resistivity was modulated as a result of carrier concentration modification, however the carrier transport process was not influenced; the Seebeck coefficient was deteriorated simultaneously. The total thermal conductivity was remarkably reduced, on account of the decreasing of phonon thermal conductivity. The thermoelectric properties of the Ba-, La-, and Ag-doped bulk samples were optimized, and the Ba-doped Ca2.9Ba0.1Co4O9 system was found to have the highest dimensionless figure of merit ZT0.20 at 973 K, which was remarkably higher than that of the un-doped sample.展开更多
基金supported by the National Basic Research Program of China (Grant No.2007CB607504)Graduate Independent Innovation Foundation of Shandong University (Grant No.yzc09076)
文摘The full-potential linear augmented plane wave method based on density functional theory is employed to investigate the electronic structure of BaSi2. With the constant relaxation time and rigid band approximation, the electrical conductivity, Seebeck coefficient and figure of merit are calculated by using Boltzmann transport theory, further eval- uated as a function of carrier concentration. We find that the Seebeck coefficient is more anisotropic than electrical conductivity. The figure of merit of BaSi2 is predicted to be quite high at room temperature, implying that optimal doping may be an effective way to improve thermoelectric properties.
基金supported by the National Natural Science Foundation of China(Grant No.11647010)the Foundation from the Higher Education and High-quality and World-class Universities(Grant No.PY201611)
文摘The electronic structure and thermoelectric(TE) properties of Mg2GexSn1-x(x = 0.25, 0.50, 0.75) solid solutions are investigated by first-principles calculations and semi-classical Boltzmann theory. The special quasi-random structure(SQS) is used to model the solid solutions, which can produce reasonable band gaps with respect to experimental results.The n-type solid solutions have an excellent thermoelectric performance with maximum zT values exceeding 2.0, where the combination of low lattice thermal conductivity and high power factor(PF) plays an important role. These values are higher than those of pure Mg2Sn and Mg2Ge. The p-type solid solutions are inferior to the n-type ones, mainly due to the much lower PF. The maximum zT value of 0.62 is predicted for p-type Mg2Ge(0.25)Sn(0.75) at 800K. The results suggest that the n-type Mg2GexSn1-x solid solutions are promising mid-temperature TE materials.
基金the National Natural Science Foundation of China(Nos.5137218 and 51521001)the 111 Project(B13035)+4 种基金the International Science&Technology Cooperation Program of China(2014DFA53090)the Natural Science Foundation of Hubei Province,China(2016CFA006)the Fundamental Research Funds for the Central Universities(WUT:2017II43GX,2017III032,2017-YB-004)the Science Challenge Project(No.TZ2016001)the State Key Laboratory of Advanced Technology for Materials Synthesis and Processing(WUT,No:2017-KF-5)
文摘The p-type Ge doped Fe0.4Co3.6Sb12-xGex skutterudites with multi-scaled impurity dots(500 nm-2 mm) were successfully prepared by using melt-quenching(MQ) and subsequent spark plasma sintering(SPS) technique. Compared with traditional method, the new technology significantly shortened the processing time from several days to less than 24 hours. The phase of impurity dots was demonstrated to be CoSb through analysis of X-ray diffraction(XRD) and energy-dispersive spectrum(EDS). Impurity dots were induced by Ge substitution of Sb in the non-equilibrium synthesized process. Due to the abandonment of the long reaction of annealing crystallization, a few of Ge atoms would fail to substitute Sb site of skutterudite in this non-equilibrium synthesized process, leading to that the multi-scaled impurity dots randomly distributed in the matrix of skutterudite Fe0.4Co3.6Sb12-xGex. The combination of multi-scaled impurity dots scattering long wavelength heat-carrying phonons and the point defect scattering short and middle wavelength heat-carrying phonons dramatically made the 22.2% reduction of lattice thermal conductivity. As a result, compared with unsubstituted sample of Fe0.4Co3.6Sb12, the maximum ZT value was increased by 30.5%. Thus, the two marked features of this new synthesis process, the shortened preparation time and the enhanced thermoelectric performance, would make a promising commercial application in the future.
基金Project supported by the National Natural Science Foundation of China(Grant No.51262032)
文摘This study prepares a group of single crystalline β-Zn_4Sb_3 with Ge and Sn codoped by the Sn-flux method according to the nominal stoichiometric ratios of Zn_(4.4)Sb_3 Ge_xSn_3(x = 0–0.15). The prepared samples possess a metallic luster surface with perfect appearance and large crystal sizes. The microscopic cracks or defects are invisible in the samples from the back-scattered electron image. Except for the heavily Ge-doped sample of x = 0.15, all the samples are single phase with space group R3c. The thermal analysis results show that the samples doped with Ge exhibit an excellent thermal stability.Compared with the polycrystalline Ge-substituted β-Zn_4Sb_3, the present single crystals have higher carrier mobility, and hence the electrical conductivity is improved, which reaches 7.48×10~4S·m^(-1) at room temperature for the x = 0.1 sample.The change of Ge and Sn contents does not improve the Seebeck coefficient significantly. Benefiting from the increased electrical conductivity, the sample with x = 0.075 gets the highest power factor of 1.45×10^(-3)W·m^(-1)·K^(-2) at 543 K.
基金Foundation item: Project supported by National Natural Science Foundation of China (50801002), Beijing Municipal Natural Science Foundation (2112007) and the Education Department of Henan Province Science and Technology Research Projects (13B430895)
文摘The Ba-, La- and Ag-doped polycrystalline Ca2.9M0.1Co4O9 (M=Ca, Ba, La, Ag) thermoelectric bulk samples were pre- pared via citrate acid sol-gel synthesis method followed by spark plasma sintering technique. The bulk samples were characterized and analyzed with regard to their phase compositions, grain orientations as well as microstructures. The high temperature thermoelec- tric transport properties of the bulk samples were studied in detail. All bulk samples were found to be single-phased with modified body texture. The electrical resistivity was modulated as a result of carrier concentration modification, however the carrier transport process was not influenced; the Seebeck coefficient was deteriorated simultaneously. The total thermal conductivity was remarkably reduced, on account of the decreasing of phonon thermal conductivity. The thermoelectric properties of the Ba-, La-, and Ag-doped bulk samples were optimized, and the Ba-doped Ca2.9Ba0.1Co4O9 system was found to have the highest dimensionless figure of merit ZT0.20 at 973 K, which was remarkably higher than that of the un-doped sample.