The microstructures at grain boundaries of SiGe, CoSb
3 and BiSb (mainly Bi) thermoelectric sintered materials have been controlled by using the plasma-treated raw powders in order to improve their thermoelectric properties. The powder surfaces of these materials were treated in the SiH
4 plasma for SiGe, the O
2 plasma for CoSb
3, and the O
2, H
2, Ar, CoSb
3+H
2 plasmas for Bi, and their thermoelectric materials were sintered by the spark plasma sintering. For the SiGe samples, the Seebeck coefficient was enhanced by using the SiH
4 plasma-treated raw powder, and the result was compared with the calculated one based on the energy filtering effect at Si-rich grain boundaries. For the CoSb
3 samples sintered using the O
2 plasma-treated raw powder, a decrease in the electrical conductivity and an increase in the Seebeck coefficient was observed, which were considered to be caused by the energy filtering effect of oxide layers at grain boundaries. The thermal conductivity was decreased. As a result, the figure of merit was improved by using the O
2 plasma-treated raw powder. For the Bi samples sintered using the O
2 plasma-treated raw powder, the electrical conductivity was increased, suggesting a decrease in the defects at grain boundaries. This result led to an improvement in the figure of merit. The room temperature values of the figure of merit were in excess of that calculated assuming that Bi single crystal grains are randomly oriented. The Bi samples sintered using other plasma-treated powders had also a higher figure of merit than that of the single crystal. For BiSb samples sintered using the O
2 plasma-treated raw powder, an increase in the electrical conductivity was also observed.
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