Sn-doped Sb2S3: p-type transition and Seebeck coefficient enhancement toward wearable thermoelectrics
摘要
Stibnite has recently emerged as a promising thermoelectric material due to its inherently low lattice thermal conductivity and high Seebeck coefficient. To make it more suitable for practical applications, enhancements in electrical transport and reductions in phonon-mediated heat transport are necessary. In this study, we substitutionally doped stibnite with tin at varying concentrations to achieve controlled phonon transport and enhanced thermoelectric properties, marking the first experimental demonstration of Sn-doped Sb2S3 for thermoelectric applications. Structural analysis via XRD confirms that Sn doping preserves the orthorhombic crystal structure, introducing lattice distortions. These structural changes significantly influence phonon transport by enhancing phonon-defect scattering. Seebeck, Hall, and thermal conductivity measurements reveal that Sn doping induces a conductivity type transition from intrinsic n-type to p-type, attributed to the substitution of Sn2+ at Sb3+ lattice sites. This substitution increases the hole concentration, leading to a substantial enhancement in the Seebeck coefficient from 341 µV/K in 2% Sn doping to a peak value of 658 µV/K at 10% Sn doping. Simultaneously, a reduction in thermal conductivity from 0.099 to 0.088 W/mK is realized, primarily due to strong phonon scattering mechanisms, including Umklapp and defect-induced scattering, which are more pronounced at higher doping levels. A wearable thermoelectric generator (WTEG) fabricated using 10% Sn-doped (p-type) and undoped (n-type) Sb2S3 generated 7.3 mV at ΔT = 2.7 °C, demonstrating its potential for self-powered wearable systems.
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