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Regioselective Zr5 Nanocluster Photocatalyst for Precise Protein Editing Under Mild Conditions.

Siqi Xie1, Stamatis S Passadis1, Mark Gray2

  • 1Department of Chemistry, KU Leuven, Celestijnenlaan 200F, Leuven, 3001, Belgium.

Angewandte Chemie (International Ed. in English)
|September 15, 2025
PubMed
Summary

A novel zirconium-oxo nanocluster (Zr5) acts as a visible-light photocatalyst for regioselective protein modification. This method enables precise oxidative cleavage and side-chain editing of proteins for proteomics applications.

Keywords:
Metal‐oxo clusterOxidationPhotocatalysisProteinZirconium oxo‐cluster

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Area of Science:

  • * Protein chemistry and chemical biology.
  • * Materials science and nanotechnology.
  • * Photocatalysis and green chemistry.

Background:

  • * Precise control over protein oxidative modifications is crucial for understanding structure-function relationships.
  • * Developing efficient and selective methods for protein editing is an ongoing challenge in biochemical research.
  • * Visible-light photocatalysis offers a promising avenue for sustainable chemical transformations.

Purpose of the Study:

  • * To develop a novel photocatalyst for regioselective protein modification.
  • * To investigate the catalytic mechanism and efficiency of a zirconium-oxo nanocluster (Zr5).
  • * To demonstrate the application of Zr5 in protein cleavage and side-chain modification for proteomics.

Main Methods:

  • * Synthesis and characterization of a novel Zr5 nanocluster.
  • * Photophysical property analysis using Time-dependent density functional theory (DFT) calculations.
  • * Visible-light photocatalysis of hen egg white lysozyme using Zr5 under 370 nm irradiation.
  • * Analysis of protein fragments using middle-down proteomics techniques.

Main Results:

  • * The Zr5 nanocluster exhibits unique photophysical properties with a low optical gap (2.01 eV).
  • * Zr5 efficiently mediates regioselective protein cleavage and oxidative side-chain modification of lysozyme under visible light.
  • * The photocatalyst demonstrates high stability and reusability without loss of catalytic activity.
  • * Reactive oxygen species generated by Zr5 are identified as key mediators of protein oxidation and cleavage.

Conclusions:

  • * The novel Zr5 nanocluster serves as an effective visible-light photocatalyst for regioselective protein editing.
  • * This approach provides a precise method for protein functionalization and fragmentation, valuable for proteomics.
  • * The findings open new avenues for utilizing zirconium-oxo clusters in molecular transformations and biocatalysis.