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<p>Semiconductor-based photoelectrochemistry commonly relies on efficient interactions between semiconductor surfaces and adsorbates for promoting charge transfer and efficiently activating inert bonds. But at the repulsive interfaces (e.g., between like-charged substrates and electrodes), such interactions cannot be achieved. Contrary to this paradigm, we find that the van der Waals interaction between a series of N-coordinated Cu complex cations and BiVO<sub>4</sub> photoanodes results in a high photovoltage of 0.53 V and charge transfer efficiency of 96%, along with the photocurrent density approaching the theoretical limit of BiVO<sub>4</sub>. This non-covalent interaction enables the universal generation of nitrogen-centered radicals from directly cleaving native N−H bonds and generates N–N coupling products with a Faradaic efficiency exceeding 96%. Its practical application is further demonstrated in an amplified photoelectrochemical reactor, generating a photocurrent of 409 mA and a yield rate of 6069 μmol h<sup>−1</sup> for hydrazine production, which is competitive with most reported N−N coupling methods.</p>

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Direct generation of nitrogen-centered radicals via non-covalent interaction between Cu complexes and BiVO4 photoanodes

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年9月30日

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  • Lei Wu,
  • Kun Dang,
  • Qiaozhen Li,
  • Yi Xu,
  • Yuchao Zhang,
  • Jincai Zhao

摘要

Semiconductor-based photoelectrochemistry commonly relies on efficient interactions between semiconductor surfaces and adsorbates for promoting charge transfer and efficiently activating inert bonds. But at the repulsive interfaces (e.g., between like-charged substrates and electrodes), such interactions cannot be achieved. Contrary to this paradigm, we find that the van der Waals interaction between a series of N-coordinated Cu complex cations and BiVO4 photoanodes results in a high photovoltage of 0.53 V and charge transfer efficiency of 96%, along with the photocurrent density approaching the theoretical limit of BiVO4. This non-covalent interaction enables the universal generation of nitrogen-centered radicals from directly cleaving native N−H bonds and generates N–N coupling products with a Faradaic efficiency exceeding 96%. Its practical application is further demonstrated in an amplified photoelectrochemical reactor, generating a photocurrent of 409 mA and a yield rate of 6069 μmol h−1 for hydrazine production, which is competitive with most reported N−N coupling methods.