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<p>Single-atom nanozymes (SAzymes) can emulate the metal active sites of natural enzymes with atomic-level precision, holding great promise as the next generation of nanozyme materials. However, the synthesis of SAzyme with high peroxidase-like activity still poses significant challenges. In this work, through precise coordination regulation of SAzymes, axial oxygen-coordinated iron SAzyme (Fe-N<sub>3</sub>O SAzyme) with high peroxidase-like activity was successfully synthesized. The synthesized Fe-N<sub>3</sub>O SAzyme shows a maximum reaction rate (<i>V</i><sub>max</sub>) of approximately 4.5 µM/min, which is approximately 12.7 times higher than that of Fe-N<sub>4</sub> with symmetric N-coordination for H<sub>2</sub>O<sub>2</sub> catalytic oxidation. Density functional theory calculations suggest that introducing axial oxygen into the Fe-N<sub>3</sub>O SAzyme modulates charge distribution and optimizes intermediate adsorption energies, thus reducing the reaction barrier. Due to its excellent peroxidase-like activity, Fe-N<sub>3</sub>O SAzyme was applied for constructing a colorimetric biosensing platform that can selectively detect and discriminate biothiols (cysteine, homocysteine, and glutathione), enabling in vitro diagnosis. This work paves a new avenue for designing SAzymes with high enzyme-like activity, offering promising potential for advanced disease diagnosis applications.</p>

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Electronic Structure Modulation of Axially-Coordinated Fe-N3O Nanozymes for Visual Biosensing

  • 期刊论文

  • 发表日期：

    2026年7月3日

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  • Rong Huang,
  • Wei Wang,
  • Wanyi Zhang,
  • Di Zhou,
  • Dongmei Deng,
  • Xiaoxia Yan,
  • Yunyi Lei,
  • Liqiang Luo

摘要

Single-atom nanozymes (SAzymes) can emulate the metal active sites of natural enzymes with atomic-level precision, holding great promise as the next generation of nanozyme materials. However, the synthesis of SAzyme with high peroxidase-like activity still poses significant challenges. In this work, through precise coordination regulation of SAzymes, axial oxygen-coordinated iron SAzyme (Fe-N3O SAzyme) with high peroxidase-like activity was successfully synthesized. The synthesized Fe-N3O SAzyme shows a maximum reaction rate (Vmax) of approximately 4.5 µM/min, which is approximately 12.7 times higher than that of Fe-N4 with symmetric N-coordination for H2O2 catalytic oxidation. Density functional theory calculations suggest that introducing axial oxygen into the Fe-N3O SAzyme modulates charge distribution and optimizes intermediate adsorption energies, thus reducing the reaction barrier. Due to its excellent peroxidase-like activity, Fe-N3O SAzyme was applied for constructing a colorimetric biosensing platform that can selectively detect and discriminate biothiols (cysteine, homocysteine, and glutathione), enabling in vitro diagnosis. This work paves a new avenue for designing SAzymes with high enzyme-like activity, offering promising potential for advanced disease diagnosis applications.