Realizing zT>2 in Environment-Friendly Monoclinic Cu2 S-Tetragonal Cu1.96 S Nano-Phase Junctions for Thermoelectrics

Angew Chem Int Ed Engl. 2022 Nov 7;61(45):e202212885. doi: 10.1002/anie.202212885. Epub 2022 Oct 7.

Abstract

Phase-junction nanocomposites, made of nanograins with the same composition but different phases, offer a platform to optimize the physiochemical performance of materials. Herein, we demonstrate a straightforward strategy to synthesize Cu2-x S phase-junction nanocomposites by retaining surface 1-dodecanethiol (DDT) ligands, in contrast to the traditional method that strips the ligands. As a result, phase junctions between a conventional monoclinic (m) phase and an unconventional metastable tetragonal (t) phase are obtained. The significantly improved power factor is obtained due to the doping of the t-phase. The phase-junction interfaces reduce thermal conductivity. Finally, surface regulation of phase junctions pushes the peak zT to 2.1 at 932 K, being the highest reported for environment-friendly metal sulfides. This work provides a paradigm to optimize thermoelectric performance by controlling phase junctions through surface-ligand tuning.

Keywords: Cu2−xS; Metastable Phase; Phase Junctions; Polymorph; Thermoelectrics.