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

Lei Wu, Kun Dang, Qiaozhen Li, Yi Xu, Yuchao Zhang () and Jincai Zhao
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Lei Wu: Chinese Academy of Sciences
Kun Dang: Chinese Academy of Sciences
Qiaozhen Li: Chinese Academy of Sciences
Yi Xu: Chinese Academy of Sciences
Yuchao Zhang: Chinese Academy of Sciences
Jincai Zhao: Chinese Academy of Sciences

Nature Communications, 2025, vol. 16, issue 1, 1-12

Abstract: Abstract 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.

Date: 2025
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DOI: 10.1038/s41467-025-63670-1

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