Abstract

While electrodeposited antimony telluride thin films with silver contents demonstrated promising thermoelectric properties, their thermal conductivity and the silver content dependence remain unknown. Here, we report the thermal conductivities of Ag3.9Sb33.6Te62.5 and AgSbTe2 thin films with controlled annealing and temperature conditions and demonstrate the impact of silver content on thermal transport. After annealing at 160 °C, the room-temperature thermal conductivity of Ag3.9Sb33.6Te62.5 and AgSbTe2 thin films increases from 0.24 to 1.59 Wm−1 K−1 and from 0.17 to 0.56 Wm−1 K−1, respectively. Using phonon transport models and X-ray diffraction measurements, we attribute the thermal conductivity increases to the crystal growth and explain the thermal conductivity variations with the degree of crystallization. Unlike electrical properties reported in previous studies, the presence of silver contents has little impact on the thermal conductivity of Ag3.9Sb33.6Te62.5 and leads to a strong reduction in the thermal conductivity of AgSbTe2 thin films. By performing transient thermal conductivity measurements at 94 °C, we find the crystallization activation energy of Ag3.9Sb33.6Te62.5 and AgSbTe2 films as 1.14 eV and 1.16 eV, respectively. Their differences reveal the role of silver in inhibiting the nucleation and growth of Sb2Te3 crystals and impeding thermal transport. These findings provide guidance for optimizing doping and annealing conditions of antimony tellurides for near-room-temperature thermoelectric applications.

Highlights

  • Nanostructured thermoelectric (TE) materials are widely studied for reducing the thermal conductivity and improving the power factor, which can increase the efficiency of thermoelectric power generators and solid-state cooling devices[1,2,3,4,5]

  • TM and Ag3.9Sb33.6Te62.5 films are investigated by X-ray Diffraction (XRD) (Smartlab, Rigaku Corp ) analysis and the average grain size is estimated based on the major XRD peaks

  • The room-temperature thermal conductivity of electrodeposited Ag3.9Sb33.6Te62.5 films is lower that of Sb37Te63 films[8] when the pre-annealing temperature is below 110 °C, and there is no significant difference when the pre-annealing temperature is above 110 °C

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Summary

Introduction

Nanostructured thermoelectric (TE) materials are widely studied for reducing the thermal conductivity and improving the power factor, which can increase the efficiency of thermoelectric power generators and solid-state cooling devices[1,2,3,4,5]. Our previous studies[6,8] demonstrated a zT of 0.35 for electrodeposited Sb37Te63 films pre-annealed at 80 °C due to the combination of low thermal conductivity and enhanced power factor provided by a secondary phase; and nanostructured Bi0.5Sb1.5Te3 achieved a zT above 1 at room temperature by inducing small grain sizes and highly dense dislocations[20,21]. Electrodeposited AgSbTe2 annealed at 100 °C demonstrated a high power factor of 553 μWm−1 K and it is expected to present a very low thermal conductivity that could lead to higher zT values[14] These power factors indicate promising materials for thermoelectric applications, which motivated a more detailed study of the thermal properties of the electrodeposited films with different compositions and annealing conditions. By comparing the thermal conductivity of SbTe films with varying silver contents and by analyzing the temperature- and time-dependent thermal conductivity data, this work provides a detailed understanding of the effects of silver content and crystallization on thermal transport

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