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<p>Photocatalysis offers a promising approach for renewable energy conversion and storage, but short lifetimes of charge-separated states in photocatalysts due to charge recombination limit its utility. Here we report an organic molecule with an acceptor–donor–acceptor configuration that can self assemble into highly crystalline nanoparticles. Transient absorption spectroscopy reveals that these crystalline assemblies can induce an ultra-long-lived charge-separated state of up to 1.2 s, attributed to initial symmetry-breaking charge separation, followed by charge hopping across closely packed molecules. These self-assembled nanoparticles have an impressive photocatalytic H<sub>2</sub> evolution rate of 126 mmol g<sup>−1</sup> h<sup>−1</sup> with an external quantum efficiency of 12% at 550 nm under optimized conditions. This system shows a remarkable stability with 220 million turnover numbers (per particle) over the 77 h of operation. These findings suggest that rational design of organic molecules and their aggregates is vital for improving light-induced charge separation and for developing highly efficient, stable and scalable organic photocatalysts.</p><p></p>

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Organic crystalline nanoparticles with a long-lived charge-separated state for efficient photocatalytic hydrogen production

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年1月20日

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  • Bin Cai,
  • Andjela Brnovic,
  • Mariia V. Pavliuk,
  • Leif Hammarström,
  • Lars Kloo,
  • Sarah A. Barnett,
  • Haining Tian

摘要

Photocatalysis offers a promising approach for renewable energy conversion and storage, but short lifetimes of charge-separated states in photocatalysts due to charge recombination limit its utility. Here we report an organic molecule with an acceptor–donor–acceptor configuration that can self assemble into highly crystalline nanoparticles. Transient absorption spectroscopy reveals that these crystalline assemblies can induce an ultra-long-lived charge-separated state of up to 1.2 s, attributed to initial symmetry-breaking charge separation, followed by charge hopping across closely packed molecules. These self-assembled nanoparticles have an impressive photocatalytic H2 evolution rate of 126 mmol g−1 h−1 with an external quantum efficiency of 12% at 550 nm under optimized conditions. This system shows a remarkable stability with 220 million turnover numbers (per particle) over the 77 h of operation. These findings suggest that rational design of organic molecules and their aggregates is vital for improving light-induced charge separation and for developing highly efficient, stable and scalable organic photocatalysts.