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<p>The photocatalytic efficiency of covalent organic frameworks is often limited by poor charge separation and inaccessible catalytic sites. Here, we overcome these challenges by constructing a biomimetic “alveoli-on-lamina” heterostructure through coordination-directed assembly. This strategy concurrently exfoliates a bulk covalent organic framework into ordered lamellae and creates atomic-scale Co-N/O bridges, anchoring high-density, atomically dispersed cobalt sites. Crucially, this architecture spontaneously generates a multi-scale electric field, integrating a strong interfacial field for charge separation with an intra-structure potential gradient for directional electron transport. This field-driven vectorial charge flow delivers electrons to the catalytic sites, enabling a competitive photocatalytic performance: a hydrogen evolution rate of 534.6 mmol g<sup>-1</sup> h<sup>-1</sup> under standard irradiation without noble metals, an apparent quantum yield of 90.2% at 500 nm, and retained stability. This work demonstrates that engineering built-in electric fields across multiple scales is a valuable paradigm for advanced solar-to-fuel conversion.</p>

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Multiscale electric fields direct charges to single-atom cobalt sites for photocatalytic H2 production

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2026年4月4日

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  • Ailing Pan,
  • Bin Liu,
  • Hong Du,
  • Chuanyi Wang,
  • Yuanyuan Che,
  • Hewen Liu,
  • Gang Zhang

摘要

The photocatalytic efficiency of covalent organic frameworks is often limited by poor charge separation and inaccessible catalytic sites. Here, we overcome these challenges by constructing a biomimetic “alveoli-on-lamina” heterostructure through coordination-directed assembly. This strategy concurrently exfoliates a bulk covalent organic framework into ordered lamellae and creates atomic-scale Co-N/O bridges, anchoring high-density, atomically dispersed cobalt sites. Crucially, this architecture spontaneously generates a multi-scale electric field, integrating a strong interfacial field for charge separation with an intra-structure potential gradient for directional electron transport. This field-driven vectorial charge flow delivers electrons to the catalytic sites, enabling a competitive photocatalytic performance: a hydrogen evolution rate of 534.6 mmol g-1 h-1 under standard irradiation without noble metals, an apparent quantum yield of 90.2% at 500 nm, and retained stability. This work demonstrates that engineering built-in electric fields across multiple scales is a valuable paradigm for advanced solar-to-fuel conversion.