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The chemical composition can directly tune the transport properties of Cu2Se liquid-like materials, including the carrier concentration, carrier mobility and superionic feature.

High-pressure technique is an effective route to synthesize thermoelectric materials and tune transport properties simultaneously. In this work, S-doped copper–selenium compounds [Formula: see text], [Formula: see text] were successfully synthesized by high-pressure and high-temperature (HPHT) technology in just 30 min. [Formula: see text] samples show layered morphology composed of abundant pores and lattice defects. The appropriate S introduction ([Formula: see text] and 0.03) can effectively enhance Seebeck coefficient and reduce the thermal conductivity of [Formula: see text]. Compared with the pure [Formula: see text] sample, [Formula: see text] exhibits a 30% lower thermal conductivity, but the decline of power factor by the distinctly increased electrical resistivity at high temperature results in a smaller zT at temperature [Formula: see text] K. The variations of thermoelectric properties are resulted from the competitive effects between S-doping and actual composition change (Cu:S). It indicates that S-doping is not so effective in improving the zT value of [Formula: see text] materials by high-pressure synthesis.

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