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<p>Cross-dehydrogenative coupling (CDC) reactions provide a facile approach for direct (hetero)aromatic C(<i>sp</i><sup>2</sup>)−C and C(<i>sp</i><sup>2</sup>)−heteroatom bond formation but conventionally rely on stoichiometric oxidants. Here we introduce single-platinum-atom-decorated graphitic carbon nitride (Pt-g-C<sub>3</sub>N<sub>4</sub>) as a recyclable heterogeneous photocatalyst for hydrogen-evolution CDC reactions between various (hetero)arenes and nucleophiles. Pt-g-C<sub>3</sub>N<sub>4</sub> exhibits exceptional stability (10 cycles) with minimal platinum leaching (&lt;0.02 ppm). Notably, the photocatalytic system showcases substantial utility and practicality in synthetic chemistry, enabling late-stage functionalization of pharmaceuticals and optoelectronic materials, and scalable (decagram) drug synthesis via a simple, in-house-built high-speed circulation flow system. Mechanistic investigations through control experiments and structural characterization elucidate the pivotal role of isolated platinum sites and substrate electronic properties in governing reaction selectivity. The integration of hydrogen-evolution CDC reactions with recyclable heterogeneous photocatalysis represents one of the greenest strategies for chemical synthesis, underscoring the promising future of single-atom catalysts as photocatalysts.</p><p></p>

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Single-atom photocatalysis boosting oxidant-free cross-dehydrogenative couplings of (hetero)arenes with nucleophiles

  • 期刊论文

  • 发表日期：

    2025年12月1日

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  • Yang Shi,
  • Xiao Hai,
  • Lei Cheng,
  • Haolin Du,
  • Xiaoye Yu,
  • Hwee Ting Ang,
  • Jiale Wu,
  • Jinxing Chen,
  • Gan Wang,
  • Jiong Lu,
  • Jie Wu

摘要

Cross-dehydrogenative coupling (CDC) reactions provide a facile approach for direct (hetero)aromatic C(sp2)−C and C(sp2)−heteroatom bond formation but conventionally rely on stoichiometric oxidants. Here we introduce single-platinum-atom-decorated graphitic carbon nitride (Pt-g-C3N4) as a recyclable heterogeneous photocatalyst for hydrogen-evolution CDC reactions between various (hetero)arenes and nucleophiles. Pt-g-C3N4 exhibits exceptional stability (10 cycles) with minimal platinum leaching (<0.02 ppm). Notably, the photocatalytic system showcases substantial utility and practicality in synthetic chemistry, enabling late-stage functionalization of pharmaceuticals and optoelectronic materials, and scalable (decagram) drug synthesis via a simple, in-house-built high-speed circulation flow system. Mechanistic investigations through control experiments and structural characterization elucidate the pivotal role of isolated platinum sites and substrate electronic properties in governing reaction selectivity. The integration of hydrogen-evolution CDC reactions with recyclable heterogeneous photocatalysis represents one of the greenest strategies for chemical synthesis, underscoring the promising future of single-atom catalysts as photocatalysts.