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<p>Due to its low cost, eco-friendliness, and excellent thermoelectric (TE) performance, copper sulfide (Cu<sub>2−<i>x</i></sub>S) has emerged as a promising TE material. Nevertheless, the trade-off between enhanced electrical conductivity and suppressed thermal conductivity is a critical challenge. This study systematically investigated an intermediate doping approach through the strategic incorporation of copper alloys (bronze, cupronickel, and brass) to optimize the TE performance of Cu<sub>1.8</sub>S. The proposed strategy realized partial copper source replacement and solved the problem of excessive Cu vacancy in Cu<sub>1.8</sub>S. Comprehensive characterization demonstrated that compared to conventional direct elemental doping, the intermediate doping with Zn, Sn, Pb, and Ni elements achieved superior TE performance. Additionally, this improvement was from dual synergistic mechanisms: the increased solubility limits facilitating optimized carrier concentration, and the <i>in situ</i> formation of the nanoscale second phase effectively scattered phonons. Ultimately, the Cu<sub>1.8</sub>S + 5 wt.% bronze + 3 wt.% cupronickel + 2 wt.% brass sample reached a remarkable <i>ZT</i> value of 1.7 at 673 K, which was a 247% enhancement over pristine Cu<sub>1.8</sub>S and surpassed all previously reported <i>ZT</i> values for the Cu<sub>1.8</sub>S system. This study established a novel paradigm of intermediate doping in optimizing the TE properties, providing a new perspective for other alloy-based TE systems.</p>

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Realizing high thermoelectric performance in copper sulfide via intermediate doping

  • 期刊论文

  • 发表日期：

    2025年6月6日

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  • Tian-Yu Yang,
  • Chong-Yu Wang,
  • Xi Yan,
  • Yi-Ming Zhang,
  • Xing Yang,
  • Wei-Hui Zhou,
  • Yi-Xin Zhang,
  • Zhen-Hua Ge,
  • Jing Feng

摘要

Due to its low cost, eco-friendliness, and excellent thermoelectric (TE) performance, copper sulfide (Cu2−xS) has emerged as a promising TE material. Nevertheless, the trade-off between enhanced electrical conductivity and suppressed thermal conductivity is a critical challenge. This study systematically investigated an intermediate doping approach through the strategic incorporation of copper alloys (bronze, cupronickel, and brass) to optimize the TE performance of Cu1.8S. The proposed strategy realized partial copper source replacement and solved the problem of excessive Cu vacancy in Cu1.8S. Comprehensive characterization demonstrated that compared to conventional direct elemental doping, the intermediate doping with Zn, Sn, Pb, and Ni elements achieved superior TE performance. Additionally, this improvement was from dual synergistic mechanisms: the increased solubility limits facilitating optimized carrier concentration, and the in situ formation of the nanoscale second phase effectively scattered phonons. Ultimately, the Cu1.8S + 5 wt.% bronze + 3 wt.% cupronickel + 2 wt.% brass sample reached a remarkable ZT value of 1.7 at 673 K, which was a 247% enhancement over pristine Cu1.8S and surpassed all previously reported ZT values for the Cu1.8S system. This study established a novel paradigm of intermediate doping in optimizing the TE properties, providing a new perspective for other alloy-based TE systems.