Bismuth telluride（Bi2Te3） based alloys, such as p-type Bi（0.5）Sb（1.5）Te3, have been leading candidates for near room temperature thermoelectric applications. In this study, Bi（0.48）Sb（1.52）Te3 bulk materials...Bismuth telluride（Bi2Te3） based alloys, such as p-type Bi（0.5）Sb（1.5）Te3, have been leading candidates for near room temperature thermoelectric applications. In this study, Bi（0.48）Sb（1.52）Te3 bulk materials with MnSb2Se4 were prepared using high-energy ball milling and spark plasma sintering（SPS） process. The addition of MnSb2Se4 to Bi（0.48）Sb（1.52）Te3 increased the hole concentration while slightly decreasing the Seebeck coefficient, thus optimising the electrical transport properties of the bulk material. In addition, the second phases of MnSb2Se4 and Bi（0.48）Sb（1.52）Te3 were observed in the Bi（0.48）Sb（1.52）Te3 matrix. The nanoparticles in the semi-coherent second phase of MnSb2Se4 behaved as scattering centres for phonons,yielding a reduction in the lattice thermal conductivity. Substantial enhancement of the figure of merit, ZT, has been achieved for Bi（0.48）Sb（1.52）Te3 by adding an Mn（0.8）Cu（0.2）Sb2Se4（2mol%） sample, for a wide range of temperatures, with a peak value of 1.43 at 375 K, corresponding to -40% improvement over its Bi（0.48）Sb（1.52）Te3 counterpart. Such enhancement of the thermoelectric（TE） performance of p-type Bi2Te3 based materials is believed to be advantageous for practical applications.展开更多
The behaviors of electrical resistivity vs temperature(ρ-T) of the molten p-type thermoelectric alloy Bi0.3Sb1.7Te3(at.%) were explored in heating and cooling processes. An obvious hump appeared on the ρ-T curve fro...The behaviors of electrical resistivity vs temperature(ρ-T) of the molten p-type thermoelectric alloy Bi0.3Sb1.7Te3(at.%) were explored in heating and cooling processes. An obvious hump appeared on the ρ-T curve from 932 ℃ to 1,020 ℃ at the heating process, while the curve became smooth in the following cooling, which suggests an irreversible temperature-induced liquid-liquid structure transition(TI-LLST) occurred in the liquid alloy. Based on this judgment, solidification experiments were carried out to find out the effects of the different liquid states. It was verified that, for the melt experiencing the presumed TI-LLST, both the nucleation and growth undercooling degrees were elevated and the solidification time was remarkably prolonged. On the other hand, the configuration of Bi0.3Sb1.7Te3 phase was refined, and its preferential orientation was weakened.展开更多
Bi_（0.5）Sb_（1.5）Te_3/Cu core/shell powders were prepared by electroless plating and hydrogen reduction, and then sintered into bulk by spark plasma sintering. After electroless plating, with increasing the Cu cont...Bi_（0.5）Sb_（1.5）Te_3/Cu core/shell powders were prepared by electroless plating and hydrogen reduction, and then sintered into bulk by spark plasma sintering. After electroless plating, with increasing the Cu content, the electrical conductivity keeps enhancing significantly. The highest electrical conductivity reaches 3341 S/cm at room temperature in Bi0.5Sb1.5Te3 with 0.67 wt% Cu bulk sample. Moreover, the lowest lattice thermal conductivity reaches 0.32 W/m·K at 572.2 K in Bi0.5Sb1.5Te3 with 0.67 wt% Cu bulk sample, which is caused by the scattering of the rich-copper particles with different dimensions and massive grain boundaries. According to the results, the ZT values of all Bi0.5Sb1.5Te3/Cu bulk samples have improved in a high temperature range. In Bi0.5Sb1.5Te3 with 0.15 wt% Cu bulk sample, the highest ZT value at 573.4 K is 0.81. When the Cu content increases to 0.67 wt%, the highest ZT value reaches 0.85 at 622.2 K. Meanwhile, the microhardness increases with increasing the Cu content.展开更多
Bi 0.5 Sb 1.5 Te 3/polyaniline composites were prepared by mechanical blending and in situ polymerization, and their transport properties were measured. It was found that for the composites with 1%, 3%, 5% and 7% poly...Bi 0.5 Sb 1.5 Te 3/polyaniline composites were prepared by mechanical blending and in situ polymerization, and their transport properties were measured. It was found that for the composites with 1%, 3%, 5% and 7% polyaniline (mass fraction) respectively, which were prepared by mechanical blending, the power factors decrease by about 30%, 50%, 55% and 65% compared with the Bi 0.5 Sb 1.5 Te 3 samples, which is mainly due to the remarkable decreases of the electrical conductivity. The electrical conductivity and power factor of the composites samples with 7% polyaniline prepared by in situ polymerization are higher by about 65% and 60%, respectively, than that of the corresponding samples prepared by mechanical blending.展开更多
To optimize the performance of a thermoelectric device for a specific application, the device should be uniquely designed for the application. Achieving an optimum design requires accurate measurements and credible an...To optimize the performance of a thermoelectric device for a specific application, the device should be uniquely designed for the application. Achieving an optimum design requires accurate measurements and credible analysis to evaluate the performance of the device and its relationship with the device parameters. To do that, we designed, fabricated, and tested four devices based on Bi2Te3 and Sb2Te3. To evaluate the accuracy of our analysis, experimental measurements were compared with the numerical simulation performed using COMSOLTM. The two sets of results were found to be in full agreement. This is a proof of the accuracy of our experimental measurements and the credibility of our simulation. The study shows that testing or simulating the devices without heat sink will lead to skewed results. This is because the junction will not hold its temperatures value, but will, instead, automatically change its value to the direction of thermal equilibrium. The study shows also that there is no reciprocity between the input and the output characteristics of the devices. Therefore, a device optimized for cooling and heating may not be automatically optimized for energy harvesting. For heating and cooling, temperature sensitivity should be optimized;while for energy harvesting, voltage sensitivity should be optimized. Using heat sink, our devices achieved a voltage sensitivity of 187.77 μV/K and a temperature sensitivity of 6.12 K/mV.展开更多
In this work, micro/nano-structured Bi0.5Sb1.5Te3bulk thermoelectric materials were synthesized by mechanical alloying from elemental shots of Bi, Sb, and Te. Cold pressing and subsequent heat treatments with hydrogen...In this work, micro/nano-structured Bi0.5Sb1.5Te3bulk thermoelectric materials were synthesized by mechanical alloying from elemental shots of Bi, Sb, and Te. Cold pressing and subsequent heat treatments with hydrogen reduction were used to form bulk solid samples with good thermoelectric properties in the temperature range around 75℃to 100℃. In comparison to crystal growth methods and chemical solution synthesis, the reported technique can be readily implemented for mass production with relatively low cost.展开更多
The investigation of the structure and thermoelectric properties of nanostructured solid solutions (Bi, Sb)2Te3 p-type has been carried out. The samples were obtained by grinding of original compositions in a planetar...The investigation of the structure and thermoelectric properties of nanostructured solid solutions (Bi, Sb)2Te3 p-type has been carried out. The samples were obtained by grinding of original compositions in a planetary ball mill and by spark plasma sintering (SPS). Initial powder has an average particle size of 10 - 12 nm according to transmission electron microscopy, and the size of the coherent scattering region (CSR) obtained by X-ray line broadening. During sintering at Ts = 250°C - 400°C, the grain size and CSR increased, which was associated with the processes of recrystallization. The maximum of size distribution of CSR shifts to larger sizes when Ts increases so that no broadening of X-ray lines at Ts = 400°C can take place. At higher Ts, the emergence of new nanograins is observed. The formation of nanograins is conditioned by reducing of quantity of the intrinsic point defects produced in the grinding of the source materials. The study of the electrical conductivity and the Hall effect in a single crystal allows to estimate the mean free path of the holes-L in the single crystal Bi0.5Sb1.5Te3 which at room temperature is 2 - 5 nm (it is much smaller than the dimensions of CSR in the samples). The method for evaluation of L in polycrystalline samples is proposed. At room temperature, L is close to the mean free path in single crystals. Scattering parameter holes in SPS samples obtained from the temperature dependence of the Seebeck coefficient are within the measurement error equal to the parameter of the scattering of holes in a single crystal. The figure of merit ZT of SPS samples as a function of composition and sintering temperature has been investigated. Maximum ZT, equal to 1.05 at room temperature, is obtained for the composition Bi0.4Sb1.6Te3 at Ts = 500°C and a pressure of 50 MPa. The causes of an apparent increase in thermoelectric efficiency are discussed.展开更多
We report on the fabrication and characterization of multi-leg bismuth telluride (Bi2Te3) and antimony telluride (Sb2Te3) thermoelectric devices. The two materials were deposited, on top of SiO2/Si substrates, using P...We report on the fabrication and characterization of multi-leg bismuth telluride (Bi2Te3) and antimony telluride (Sb2Te3) thermoelectric devices. The two materials were deposited, on top of SiO2/Si substrates, using Pulsed Laser Deposition (PLD). The SiO2 layer was used to provide insulation between the devices and the Si wafer. Copper was used as an electrical connector and a contact for the junctions. Four devices were built, where the Bi2Te3 and Sb2Te3 were deposited at substrate temperatures of 100°C, 200°C, 300°C and 400°C. The results show that the device has a voltage sensitivity of up to 146 μV/K and temperature sensitivity of 6.8 K/mV.展开更多
基金supported by the National Natural Science Foundation of China(Grant Nos.51472052 and Y6J1421A41)
文摘Bismuth telluride（Bi2Te3） based alloys, such as p-type Bi（0.5）Sb（1.5）Te3, have been leading candidates for near room temperature thermoelectric applications. In this study, Bi（0.48）Sb（1.52）Te3 bulk materials with MnSb2Se4 were prepared using high-energy ball milling and spark plasma sintering（SPS） process. The addition of MnSb2Se4 to Bi（0.48）Sb（1.52）Te3 increased the hole concentration while slightly decreasing the Seebeck coefficient, thus optimising the electrical transport properties of the bulk material. In addition, the second phases of MnSb2Se4 and Bi（0.48）Sb（1.52）Te3 were observed in the Bi（0.48）Sb（1.52）Te3 matrix. The nanoparticles in the semi-coherent second phase of MnSb2Se4 behaved as scattering centres for phonons,yielding a reduction in the lattice thermal conductivity. Substantial enhancement of the figure of merit, ZT, has been achieved for Bi（0.48）Sb（1.52）Te3 by adding an Mn（0.8）Cu（0.2）Sb2Se4（2mol%） sample, for a wide range of temperatures, with a peak value of 1.43 at 375 K, corresponding to -40% improvement over its Bi（0.48）Sb（1.52）Te3 counterpart. Such enhancement of the thermoelectric（TE） performance of p-type Bi2Te3 based materials is believed to be advantageous for practical applications.
基金financially supported by the National Natural Science Foundation of China(grant no.51371073)the Research Fund for the Doctoral Program of Higher Education of China(20110111110014)the National Basic Research Program of China(grant no.2012CB825702)
文摘The behaviors of electrical resistivity vs temperature(ρ-T) of the molten p-type thermoelectric alloy Bi0.3Sb1.7Te3(at.%) were explored in heating and cooling processes. An obvious hump appeared on the ρ-T curve from 932 ℃ to 1,020 ℃ at the heating process, while the curve became smooth in the following cooling, which suggests an irreversible temperature-induced liquid-liquid structure transition(TI-LLST) occurred in the liquid alloy. Based on this judgment, solidification experiments were carried out to find out the effects of the different liquid states. It was verified that, for the melt experiencing the presumed TI-LLST, both the nucleation and growth undercooling degrees were elevated and the solidification time was remarkably prolonged. On the other hand, the configuration of Bi0.3Sb1.7Te3 phase was refined, and its preferential orientation was weakened.
基金National Natural Science Foundation of China(11834012,51620105014,51572210,51521001)National Key Research and Development Plan of China(2018YFB0703600)
基金the National Natural Science Foundation of China(No.51371073)
文摘Bi_（0.5）Sb_（1.5）Te_3/Cu core/shell powders were prepared by electroless plating and hydrogen reduction, and then sintered into bulk by spark plasma sintering. After electroless plating, with increasing the Cu content, the electrical conductivity keeps enhancing significantly. The highest electrical conductivity reaches 3341 S/cm at room temperature in Bi0.5Sb1.5Te3 with 0.67 wt% Cu bulk sample. Moreover, the lowest lattice thermal conductivity reaches 0.32 W/m·K at 572.2 K in Bi0.5Sb1.5Te3 with 0.67 wt% Cu bulk sample, which is caused by the scattering of the rich-copper particles with different dimensions and massive grain boundaries. According to the results, the ZT values of all Bi0.5Sb1.5Te3/Cu bulk samples have improved in a high temperature range. In Bi0.5Sb1.5Te3 with 0.15 wt% Cu bulk sample, the highest ZT value at 573.4 K is 0.81. When the Cu content increases to 0.67 wt%, the highest ZT value reaches 0.85 at 622.2 K. Meanwhile, the microhardness increases with increasing the Cu content.
文摘Bi 0.5 Sb 1.5 Te 3/polyaniline composites were prepared by mechanical blending and in situ polymerization, and their transport properties were measured. It was found that for the composites with 1%, 3%, 5% and 7% polyaniline (mass fraction) respectively, which were prepared by mechanical blending, the power factors decrease by about 30%, 50%, 55% and 65% compared with the Bi 0.5 Sb 1.5 Te 3 samples, which is mainly due to the remarkable decreases of the electrical conductivity. The electrical conductivity and power factor of the composites samples with 7% polyaniline prepared by in situ polymerization are higher by about 65% and 60%, respectively, than that of the corresponding samples prepared by mechanical blending.
文摘To optimize the performance of a thermoelectric device for a specific application, the device should be uniquely designed for the application. Achieving an optimum design requires accurate measurements and credible analysis to evaluate the performance of the device and its relationship with the device parameters. To do that, we designed, fabricated, and tested four devices based on Bi2Te3 and Sb2Te3. To evaluate the accuracy of our analysis, experimental measurements were compared with the numerical simulation performed using COMSOLTM. The two sets of results were found to be in full agreement. This is a proof of the accuracy of our experimental measurements and the credibility of our simulation. The study shows that testing or simulating the devices without heat sink will lead to skewed results. This is because the junction will not hold its temperatures value, but will, instead, automatically change its value to the direction of thermal equilibrium. The study shows also that there is no reciprocity between the input and the output characteristics of the devices. Therefore, a device optimized for cooling and heating may not be automatically optimized for energy harvesting. For heating and cooling, temperature sensitivity should be optimized;while for energy harvesting, voltage sensitivity should be optimized. Using heat sink, our devices achieved a voltage sensitivity of 187.77 μV/K and a temperature sensitivity of 6.12 K/mV.
文摘In this work, micro/nano-structured Bi0.5Sb1.5Te3bulk thermoelectric materials were synthesized by mechanical alloying from elemental shots of Bi, Sb, and Te. Cold pressing and subsequent heat treatments with hydrogen reduction were used to form bulk solid samples with good thermoelectric properties in the temperature range around 75℃to 100℃. In comparison to crystal growth methods and chemical solution synthesis, the reported technique can be readily implemented for mass production with relatively low cost.
文摘The investigation of the structure and thermoelectric properties of nanostructured solid solutions (Bi, Sb)2Te3 p-type has been carried out. The samples were obtained by grinding of original compositions in a planetary ball mill and by spark plasma sintering (SPS). Initial powder has an average particle size of 10 - 12 nm according to transmission electron microscopy, and the size of the coherent scattering region (CSR) obtained by X-ray line broadening. During sintering at Ts = 250°C - 400°C, the grain size and CSR increased, which was associated with the processes of recrystallization. The maximum of size distribution of CSR shifts to larger sizes when Ts increases so that no broadening of X-ray lines at Ts = 400°C can take place. At higher Ts, the emergence of new nanograins is observed. The formation of nanograins is conditioned by reducing of quantity of the intrinsic point defects produced in the grinding of the source materials. The study of the electrical conductivity and the Hall effect in a single crystal allows to estimate the mean free path of the holes-L in the single crystal Bi0.5Sb1.5Te3 which at room temperature is 2 - 5 nm (it is much smaller than the dimensions of CSR in the samples). The method for evaluation of L in polycrystalline samples is proposed. At room temperature, L is close to the mean free path in single crystals. Scattering parameter holes in SPS samples obtained from the temperature dependence of the Seebeck coefficient are within the measurement error equal to the parameter of the scattering of holes in a single crystal. The figure of merit ZT of SPS samples as a function of composition and sintering temperature has been investigated. Maximum ZT, equal to 1.05 at room temperature, is obtained for the composition Bi0.4Sb1.6Te3 at Ts = 500°C and a pressure of 50 MPa. The causes of an apparent increase in thermoelectric efficiency are discussed.
文摘We report on the fabrication and characterization of multi-leg bismuth telluride (Bi2Te3) and antimony telluride (Sb2Te3) thermoelectric devices. The two materials were deposited, on top of SiO2/Si substrates, using Pulsed Laser Deposition (PLD). The SiO2 layer was used to provide insulation between the devices and the Si wafer. Copper was used as an electrical connector and a contact for the junctions. Four devices were built, where the Bi2Te3 and Sb2Te3 were deposited at substrate temperatures of 100°C, 200°C, 300°C and 400°C. The results show that the device has a voltage sensitivity of up to 146 μV/K and temperature sensitivity of 6.8 K/mV.
