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<p>Plasmon-induced hot energy in metal nanostructures holds great promise for photocatalytic organic conversions. However, maintaining the high-energy state of hot electrons within these structures remains challenging, even in hybrid metal-semiconductor heterojunctions. The rapid relaxation of hot electrons (&lt; 1 ps) due to a thick-shell and loosely bound semiconductor layer limits their extraction efficiency and utilization effectiveness during photocatalysis. Herein, we fabricated a novel metal-semiconductor heterojunction <b>(P2-Au)</b> with ultrathin-shell semiconductor layer by combing ultra-small metal chalcogenide semiconductor clusters <b>(P2)</b> with gold nanorods <b>(AuNRs)</b>, which exhibits high-efficiency extraction of hot electrons and photocatalytic application. The robust binding of <b>P2</b> cluster, with its smaller volume and larger energy level splitting compared to large-sized quantum dots, not only significantly increases the yield of hot electrons but also enables their rapid extraction and sustains long-lived (&gt; 2 ns) high-energy states. As a proof of concept, the composite photocatalyst achieves near-infrared-light-driven C(sp<sup>3</sup>)–S cross-coupling reactions for the first time. This protocol effectively produces over 50 alkylthioethers from a wide scope range of non-active alkyl bromides and chlorides, aryl and alkyl thiols. This work provides a new strategy for high-efficiency extraction of hot electrons within plasmonic metal nanostructures and paves the way for hot electron-driven photo-catalytic organic transformations.</p>

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Semiconductor clusters enable high-efficiency extraction of hot electrons from gold nanorods for photocatalytic organic conversions

  • 期刊论文

  • 发表日期：

    2025年2月6日

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  • Jia-Xing Liu,
  • Hao Ma,
  • Shang-Fu Yuan,
  • Jing-Ni Zhang,
  • Jing-Guan Liang,
  • Rui Zhou,
  • Dong-Sheng Li,
  • Wenbin Chen,
  • Ming-De Li,
  • Tao Wu

摘要

Plasmon-induced hot energy in metal nanostructures holds great promise for photocatalytic organic conversions. However, maintaining the high-energy state of hot electrons within these structures remains challenging, even in hybrid metal-semiconductor heterojunctions. The rapid relaxation of hot electrons (< 1 ps) due to a thick-shell and loosely bound semiconductor layer limits their extraction efficiency and utilization effectiveness during photocatalysis. Herein, we fabricated a novel metal-semiconductor heterojunction (P2-Au) with ultrathin-shell semiconductor layer by combing ultra-small metal chalcogenide semiconductor clusters (P2) with gold nanorods (AuNRs), which exhibits high-efficiency extraction of hot electrons and photocatalytic application. The robust binding of P2 cluster, with its smaller volume and larger energy level splitting compared to large-sized quantum dots, not only significantly increases the yield of hot electrons but also enables their rapid extraction and sustains long-lived (> 2 ns) high-energy states. As a proof of concept, the composite photocatalyst achieves near-infrared-light-driven C(sp3)–S cross-coupling reactions for the first time. This protocol effectively produces over 50 alkylthioethers from a wide scope range of non-active alkyl bromides and chlorides, aryl and alkyl thiols. This work provides a new strategy for high-efficiency extraction of hot electrons within plasmonic metal nanostructures and paves the way for hot electron-driven photo-catalytic organic transformations.