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Cr-doped higher manganese silicides (HMSs) (Mn1-xCrx)Si1.75 (x = 0–0.35) have been prepared by repeated sintering from raw elemental powder using spark plasma sintering. The a- and cMn-axis length increases with increasing Cr content x. The results of powder X-ray diffraction and microstructural observation suggest that impurity phases, e.g. (Mn, Cr)Si and CrSi2, exist in the samples with x = 0.20 or above. The electrical resistivities and Seebeck coefficient decrease with increasing Cr content x. The Cr content x of 0.10 indicated the largest power factor at 850 K (1.39×10-3W/mK), followed in order by x of 0.25, 0, 0.05, 0.15, 0.20. To confirm the effect of Cr-doping on outputs of modules, two paired p-n modules consisting of n-type purchased Mg2Si and p-type Cr-doped HMS with x = 0, 0.05, 0.10, and 0.20 elements were prepared. The module consisting of (Mn0.9Cr0.1)Si1.75 showed the highest output, that is, 845 mW at 873 K on the hot side. There was approximately 8% improvement compared with that of the module consisting of Cr-free elements.
We applied NiSi2 as an electrode for thermoelectric modules because NiSi2 has high electric conductivity and is expected to suppress the inter-diffusion of Si from MgSi2 and higher manganese silicide (HMS). The thermal expansion coefficient of NiSi2 is close to that of Mg2Si but differs from that of HMS. Therefore, to reduce thermal stress, we tried to insert a buffer layer consisting of HMS and NiSi2 for the interface between the HMS sintered body and the NiSi2 electrode. The NiSi2 was prepared by using spark plasma sintering (SPS) equipment. NiSi2 electrodes and gradients were formed and connected with the HMS by SPS treatment. Crack-free bonding was achieved by inserting gradients consisting of HMS and NiSi2. The inserted composite buffer layer reduced interface stress and interface resistance between HMS and NiSi2.
The magnesium compound Mg2Si and its solid solutions are expected as n-type thermoelectric (TE) material because they are non-toxic, have a large Clarke number, and are light weight. In this study, we improved TE performance by doping Ge into Sb-doped Mg2Si to cause phonon scattering and increase carrier concentration. A bulk of Sb-doped Si-Ge alloy as the raw material was fabricated using an arc-melting method. A high-purity Mg2Si was synthesized from metal Mg and Sb-doped Si-Ge alloy using spark plasma sintering equipment. For the samples with the same Sb concentration, the electrical conductivity was equivalent. On the other hand, the Seebeck coefficient was dependent on Ge concentration. Due to phonon scattering, thermal conductivity decreased by a small amount of Ge doping and κph dominated for thermal conduction. The minimum thermal conductivity of Mg2Si0.90Ge0.10 was 2.25 W/mK (κph: 2.06 W/mK, κel: 0.19 W/mK). The dimensionless figure of merit (ZT) for the Mg2Si0.945Ge0.05Sb0.005 sample was higher than that of the others due to reducing thermal conductivity and increasing carrier concentration. The maximum ZT was 0.47 at 713 K.
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.
Complex Metallic Alloys (CMAs) are metallic solids of high structural complexity, consisting of large numbers of atoms in their unit cells. Consequences of this structural complexity are manifold and give rise to a variety of exciting physical properties. The impact that such structural complexity may have on the lattice dynamics will be discussed. The surprising dynamical flexibility of Tsai-type clusters with the symmetry breaking central tetrahedron will be addressed for Zn6Sc, while in the Ba-Ge-Ni clathrate system the dynamics of encaged Ba guest atoms in the surrounding Ge-Ni host framework is analysed with respect to the experimentally evidenced strong reduction of lattice thermal conductivity. For both systems experimental results from neutron scattering are analyzed and interpreted on atomistic scale by means of ab initio and molecular dynamics simulations, resulting in a picture with the respective structural building blocks as the origin of the peculiarities in the dynamics.
Magnetization behavior of Nd9(Fe, B)87Zr2Nb2 nanostructure magnets have been investigated. We will show that the nanostructure magnets are composed of magnetic clusters of exchange-coupled single domains and the coercivity is governed by coupling intensity between soft and hard magnetic clusters in the magnets.
Platinum nanoparticles stabilized by linear polyethyleneimine were prepared by the liquid-phase reduction of chloroplatinic(IV) acid with sodium borohydride. The particle sizes were 3.26 nm and 1.76 nm when the molecular weights of linear polyethyleneimine were 25000 and 2150, respectively. These nanoparticles were well-dispersed in water in the range of pH 1-6. Branched polyethyleneimine also provided nanoparticles that dispersed in water in the range of pH 0-8. Linear poly(ethyleneimine-co-N-methylethyleneimine) gave nanoparticles that dispersed in water in the range of pH 0-10. The dispersibility of the nanoparticles decreased with increasing content of the N-methyl group.
We have prepared a number of Pt-TM(transition metals) alloys with various TM elements and evaluated their catalytic abilities by means of hydrogenation of methyl acrylate. High catalytic activities are obtained when the crystalline structures are similar, i.e., fcc structure, indicating that the crystal structure of a catalyst plays an important role in hydrogenation of methyl acrylate. Furthermore, for a certain TM element, i.e., Mo, the catalytic activity is found to surpass that of Pt metal.
Platinum nanoparticles were dispersed in mesopores of mesoporous silica using a sol-gel process with a composite template consisting of an amphiphilic triblock copolymer (Pluronic P123 or F127) and a Pt-organic complex, which was prepared with K2Pt(II)Cl4 as a Pt source and 1,10-phenanthroline as a chelating agent. The obtained Pt-1,10-phenanthroline complex did not dissolve in any of several solvents, e.g., hexane, benzene, toluene, THF, H2O, CH3OH, and C2H5OH. However, when the Pt-1,10-phenanthroline complex was reacted with ethylenediamine it dissolved in many solvents. Platinum nanoparticles dispersed in mesoporous silica were obtained using a sol-gel process with a complex template consisting of Pt-1,10-phenanthroline-ethylenediamine, and an amphiphilic triblock copolymer (Pluronic P123 or F127). A sample dried at 353 K was bright yellow. When it was subsequently heat-treated at 823 K, it turned light gray. This change indicates that Pt nanoparticles can be obtained by heat-treatment at high temperature, because, to generate Pt nanoparticles, the organics chelated to Pt ions must be removed. Measurements from small-angle x-ray scattering show that mesoporous silica obtained using a complex template has a much more highly ordered pore structure than that obtained using only an amphiphilic triblock copolymer. It has both large pores (above 8 nm) and a large surface area (about 290 m2/g). Furthermore, results of a TEM investigation showed that Pt nanoparticles were generated only in mesopores of mesoporous silica.
The developments of high performance magnetic materials are required in various applications such as high sensitive magnetic sensing and hyperthermia in cancer treatment. Recently, Co-doped TiO2 has been received considerable attention as a candidate for such materials because of their ferromagnetic properties at room temperature. On the other hand, the phase-separated glasses and the derived glass-ceramics having unique micro-nano structure are utilized for various applications. In this study, the phase separated glass-ceramics in CoO-TiO2-SiO2 system with Al2O3 addition were prepared by melt-quenching process. The as-quenched samples consisted of the TiO2-rich phase and the SiO2-rich one which were formed by a nucleation-growth mechanism of phase separation. From the results of XRD measurements, the samples were found to have a TiO2 crystalline phase and a SiO2-rich glassy phase. The samples showed the magnetic property, which were regarded as a mixture of ferromagnetic and paramagnetic phases. The samples also showed the electric conductivity at room temperature. However, the conductivity of the sample decreased with increase of the Co content, and the temperature dependence of the conductivity of the ferromagnetic samples was different from the other ones. As a result, the Co ions in the phase-separated glass-ceramics in TiO2-SiO2 system were found to affect on both the magnetic and the electric conductive characteristics.
We have prepared Nd2Fe14B/Fe3B bulk nanocomposite magnets at the compositions of Nd4Fe77.5B18.5-xMx (M=Si, C) by substitution of other elements M for B. For the sample substituted with 1 at.%Si and sintered at 600 oC, the coercivity exhibits the highest value of 227 kA/m. It has also been found that the grain sizes of the Nd2Fe14B and the Fe3B phases depend on the ramp-up time and the reduction of the grain size leads to an increase of the coercivity. On the other hand, the samples substituted with C exhibit soft magnetic behaviors, which is attributed to the suppression of the precipitation of the Nd2Fe14B hard magnetic phase.
We report the electrical resistivity of the ternary Ag-In-(Yb,Ca) quasicrystals (QCs) together with those of their 1/1 and 2/1 cubic approximants. The temperature coefficient of the resistivity (TCR) is negative and nearly the same for the QCs and the 2/1 approximants suggesting that the coherence length of the conduction electrons in the QCs is comparable to the lattice parameter of the 2/1 approximants, i.e., ∼2.5 nm. On the other hand, both positive and negative values of TCR are observed for the 1/1 approximants depending on the annealing temperature. Taking into consideration the occurrence of positive TCR in the binary Cd-(Yb,Ca) 1/1 approximant, the latter phenomenon suggests that the negative TCR of the ternary 1/1 approximants is due to chemical disorder between Ag and In, and the chemical disorder is possibly reduced when annealed at low temperatures.
Bulk metallic glasses have extremely high strength and high ductility and are quite useful as the structural material. Many of bulk metallic glasses are based on Zr, Ti and Pd; these elements have a high affinity with hydrogen and hence the bulk metallic glasses can contain a large amount of hydrogen atoms. It is known that hydrogenized amorphous metals, as well as hydrogenized metallic crystals, exhibit Snoek-type relaxation, and hence metallic glasses containing a high density of hydrogen can have a high internal friction.
In the present experiments, internal friction measurements have been performed for bulk metallic glasses doped with a variety of hydrogen concentrations. It is shown that the peak value of the internal friction reaches the order of 10-2 in Zr-based bulk metallic glasses which have the fracture strength as high as 1.5 GPa. Thus, hydrogen-doped bulk metallic glasses can be used as the high-strength, high-damping material.
In order to gain an insight into the role of the local atomic environment in the electronic transport of the icosahedral quasicrystal, the electrical resistivity of α-AlReSi, which is the (1/1,1/1,1/1) approximant of the icosahedral phase, has been investigated. Very high resistivity and its pronounced negative temperature dependence have been observed, indicating that the electronic states of the 1/1 cubic approximant are quite similar to those of icosahedral phases. In order to further elucidate which structural entity is responsible for such anomalous transport, a comparison of the electrical resistivity between (1/1,1/1,1/1) and (1/0,1/0,1/0) approximants has been made. The typical transport behavior of icosahedral phases which is also seen in 1/1 and higher-order approximants was not observed in any of the studied 1/0 cubic approximants. The result can be regarded as an implication that the intercluster distance between the TM clusters plays a significant role in the confinement of electronic states.
In order to gain insight into the influences of formation of an icosahedral phase in Zr-based metallic glasses on the physical properties, thermal and electrical properties of Zr70Ni10Pd20 metallic glass were investigated. From DSC analyses, activation energies for the phase transition from an amorphous to an icosahedral phase and from the icosahedral to a crystalline (Zr2Ni) phase were estimated to be 3.42 and 3.07 eV, respectively. The effect of the phase transformations on the electrical resistivity was successfully observed; the resistivity clearly exhibits an increase and a decrease corresponding to the transitions from the amorphous to the icosahedral phase and from the icosahedral to the crystalline Zr2Ni phase, respectively. It is concluded that the increase of the resistivity upon the precipitation of the icosahedral phase is due to an increase of the volume fraction of the icosahedral grains, which possess higher resistivity.
Modulated photocurrent method originally developed for analyzing the electronic states of semiconductor has been applied to an Al-Pd-Re quasicrystal having high electrical resistivity. The measured DC component of the photocurrent has indicated that the mobility of the photocarrier is approximately the same as that of the dark carrier at the Fermi level. The data of the amplitude and phase shift of the AC component can be explained well by a simple model in which only the two processes, carrier generation and recombination, are involved. The recombination time obtained by fitting is by about six orders larger than those reported for semiconductors. The long recombination time as well as the energy independent mobility of carriers are discussed in view of a spiky structure in electron density of states expected for the quasicrystals.
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