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<p>The development of materials with high photocatalytic efficiency is essential for sustainable chemical transformations. Here we introduce photochargeable zinc indium sulfide nanocrystals with notable charge storage capacity, enabling highly efficient photocatalytic dehydrogenative coupling of amines. Combined with a nickel cocatalyst, the nanocrystals deliver diamines and hydrogen at rates exceeding 120 mmol per gram of photocatalyst per hour, with &gt; 95% selectivity and an apparent quantum efficiency of up to 39.4% under ambient conditions. The system exhibits excellent scalability, demonstrated by a reaction on a 20-g scale, and broad versatility in promoting amino acid ester coupling and polymerization reactions with concurrent hydrogen evolution. Mechanistic studies attribute the photocharging capability of zinc indium sulfide nanocrystals to in situ-generated trap states such as sulfur vacancies, which extend hydrogen production into the dark catalytic cycle and enhance the overall charge utilization efficiency. These findings position photochargeable semiconductors as promising platforms for a wide range of photocatalytic applications.</p><p></p>

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A photochargeable semiconductor for highly efficient dehydrogenative coupling of amines

  • 期刊论文

  • 发表日期：

    2026年3月30日

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  • Jie Luo,
  • Xinyu Chen,
  • Lihini Jayasinghe,
  • Nathan Edward Soland,
  • Yu Shan,
  • Arifin Luthfi Maulana,
  • Heqing Zhu,
  • Maria Fonseca Guzman,
  • Alexander M. Oddo,
  • Kiran M. Donnelly,
  • Jihoon Choi,
  • Julian Feijoo,
  • Bernd Schaefer,
  • Matthias Schmalzbauer,
  • Rui Zhang,
  • Fabian Seeler,
  • Carlos Lizandara-Pueyo,
  • Richard D. Schaller,
  • Peidong Yang

摘要

The development of materials with high photocatalytic efficiency is essential for sustainable chemical transformations. Here we introduce photochargeable zinc indium sulfide nanocrystals with notable charge storage capacity, enabling highly efficient photocatalytic dehydrogenative coupling of amines. Combined with a nickel cocatalyst, the nanocrystals deliver diamines and hydrogen at rates exceeding 120 mmol per gram of photocatalyst per hour, with > 95% selectivity and an apparent quantum efficiency of up to 39.4% under ambient conditions. The system exhibits excellent scalability, demonstrated by a reaction on a 20-g scale, and broad versatility in promoting amino acid ester coupling and polymerization reactions with concurrent hydrogen evolution. Mechanistic studies attribute the photocharging capability of zinc indium sulfide nanocrystals to in situ-generated trap states such as sulfur vacancies, which extend hydrogen production into the dark catalytic cycle and enhance the overall charge utilization efficiency. These findings position photochargeable semiconductors as promising platforms for a wide range of photocatalytic applications.