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Thermoelectric (TE) power generation is considered a valuable energy resource to mitigate the global energy dilemma, by converting ‘waste heat’ into ‘useful electrical energy’. Practical implementation of TE technology demands cost-effective and environmentally friendly, high-performance TE materials. To date, lead chalcogenides have been established as one of the leading candidates for TE power generation applications. However, the toxicity of Pb limits their mass market applications. Recently, Pb-free group IV–VI metal chalcogenides have attracted significant interest in the field of thermoelectrics as some, namely the chalcogenides of tin and germanium, display exceptionally high TE figures of merit, owing to their intriguing crystal and electronic structures. This chapter describes cutting-edge methodologies for the design of high-performance TE materials based on the Pb-free IV–VI class of metal chalcogenides, through improvement of the Seebeck coefficient and by effecting a decrease in the lattice thermal conductivity. The principal difficulties and future possibilities for further improvement of the TE performance of these materials are also discussed.

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