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In this study, we fabricated Mg2Si from metal Mg and Si with different particle sizes (425 - 300, 300 - 180, and 75 μm or less) using spark plasma sintering (SPS) equipment. Additionally, the Mg2Si formation was investigated. A sieved Si powder was mixed with metal Mg powder in an inert gas (Ar) atmosphere. The mixture was placed in a graphite die while still in an Ar atmosphere and subjected to SPS at 923 K and 1113 K. The obtained sintering bodies were Mg2Si particles with a size of about 5 μm. Then, the sintered bodies were evaluated by X-ray diffraction (XRD). As a result, it was confirmed that generation of Mg2Si increased with decreasing Si particle size.
Magnesium silicide (Mg2Si) has attracted much interest as an n-type thermoelectric material because it is eco-friendly, non-toxic, light, and relatively abundant compared with other thermoelectric materials. In this study, we tried to improve the thermoelectric performance by doping Sb and Ge in the Mg2Si, as well as further optimizing x in the carrier concentration to cause phonon scattering. A high purity Mg2Si was synthesized from metal Mg and Sb doped Si-Ge alloy by using spark plasma sintering (SPS) equipment. The sintered samples were cut and polished. They were evaluated by using X-ray diffraction (XRD) and X-ray fluorescence (XRF) analyses. The carrier concentration of the samples was measured by using Hall measurement equipment. The electrical conductivity and Seebeck coefficient were measured by using a standard four-probe method in a He atmosphere. The thermal conductivity was measured by using a laser-flash system. We succeeded in obtaining a Sb doped Mg2Si0.95Ge0.05 sintered body easily without any impurities with the SPS equipment. The electrical conductivity of the sample was increased, and thermal conductivity was decreased by increasing the amount of doped Sb. The dimensionless figure of merit ZT became 0.74 at 733 K in the Mg2Si0.95-xGe0.05Sbx sample with x = 0.0022.
NaxCoO2 has a particularly high contact resistance because it forms an insulated layer of NaHCO3 and Na2CO3, which are produced in a chemical reaction with carbon dioxide and water in air on the surface. In this study, we tried to improve the interface resistance between NaxCoO2 and Ag sheet electrodes by connecting these materials with the spark plasma sintering (SPS) technique. The interface resistance between NaxCoO2 and Ag sheet electrodes connected by SPS is compared with that connected with Ag paste. In an experiment, the interface resistance of a sample treated by decrease to less than 1/600 of the former value. It is thought that the NaHCO3 and Na2CO3 insulated layer is decomposed through the application of a large value of applied DC current by using the SPS technique.
Mg2Si bulk was fabricated by spark plasma sintering (SPS) nano-powder, and the thermoelectric characteristics of the bulk sample were evaluated at temperatures up to 873 K. A pre-synthesized all-molten commercial polycrystalline Mg2Si source (un-doped n-type semiconductor) was pulverized into powder of 75 μm or less. To obtain nano-sized fine powder, the powder was milled using planetary ball mill equipment under an inert atmosphere. Fine Mg2Si nano-powder with a mean grain size of about 500 nm was obtained. XRD analysis confirmed that no MgO existed in the nano-powder. The fine powder was put in a graphite die to obtain a sintering body of Mg2Si and treated by SPS under vacuum conditions. The resulting Mg2Si bulk had high density and did not crack. However, the XRD analysis revealed a small amount of MgO in it. The thermoelectric properties (electrical conductivity, Seebeck coefficient, and thermal conductivity) were measured from room temperature to 873 K. The microstructure of the sintered body was observed by scanning electron microscopy. The maximum dimensionless figure of merit of a sample made from Mg2Si nano-powder was ZT = 0.67 at 873 K.
Thermoelectric power generation has been attracting attention as a technology for waste heat utilization in which thermal energy is directly converted into electric energy. It is well known that layered cobalt oxide compounds such as NaCo2O4 and Ca3Co4O9 have high thermoelectric properties in p-type oxide semiconductors. However, in most cases, the thermoelectric properties in n-type oxide materials are not as high. Therefore, n-type magnesium silicide (Mg2Si) has been studied as an alternative due to its non-toxicity, environmental friendliness, lightweight property, and comparative abundance compared with other TE systems. In this study, we fabricated π-structure thermoelectric power generation devices using p-type NaCo2O4 elements and n-type Mg2Si elements. The p- and n-type sintering bodies were fabricated by spark plasma sintering (SPS). To reduce the resistance at the interface between elements and electrodes, we processed the surface of the elements before fabricating the devices. The end face of a Mg2Si element was covered with Ni by SPS and that of a NaCo2O4 element was coated with Ag by silver paste and soldering.
The thermoelectric device consisted of 18 pairs of p-type and n-type legs connected with Ag electrodes. The cross-sectional and thickness dimensions of the p-type elements were 3.0 mm × 5.0 mm × 7.6 mm (t) and those of the n-type elements were 3.0 mm × 3.0 mm × 7.6 mm (t). The open circuit voltage was 1.9 V and the maximum output power was 1.4 W at a heat source temperature of 873 K and a cooling water temperature of 283 K in air.
The thermoelectrical properties of α and γ phases of NaxCo2O4 having different amounts of Na were evaluated. The γ NaxCo2O4 samples were synthesized by thermal decomposition in a metal-citric acid compound, and the α NaxCo2O4 samples were synthesized by self-flux processing. Dense bulk ceramics were fabricated using spark plasma sintering (SPS), and the sintered samples were of high density and highly oriented. The thermoelectrical properties showed that γ NaxCo2O4 had higher electrical conductivity and lower thermal conductivity compared with α NaxCo2O4 and that α NaxCo2O4 had a larger Seebeck coefficient. These results show that γ NaxCo2O4 has a larger power factor and dimensionless figure of merit, ZT, than α NaxCo2O4.
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