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TiCoSb-based half-Heusler compounds have been prepared and their thermoelectric properties are studied. By isoelectronic alloying on the Ti site with Zr, although both the thermal conductivity and electrical conductivity are suppressed, the Seebeck coefficient is improved remarkably with a highest value of -420 μV/K for Ti0.5Zr0.5CoSb at 600 K, which provides a larger space to optimize the thermoelectric performance. To further improve the performance of the TiCoSb-based isoelectronic alloy, doping Ni on the Co site was explored. It is found that small amount of Ni doping results in a great increase in the electrical conductivity, still with a relative large Seebeck coefficient. Ti0.6Hf0.4Co0.87Ni0.13Sb sample exhibits a peak power factor of 23.4 μW/cm K2, which is the highest value for n-type TiCoSb-based half-Heusler compounds reported so far. As a result, a maximum dimensionless figure of merit of 0.70 has been achieved at 900 K for Ti0.6Hf0.4Co0.87Ni0.13Sb. [ABSTRACT FROM AUTHOR]