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Multidimensional Engineering of Single-Atom Iron Nanozymes for Machine Learning-Assisted Multiplexed Sensing.

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We engineered iron single-atom nanozymes with novel multidimensional coordination for enhanced H2O2 activation. This breakthrough enables sensitive detection of tetracycline antibiotics in water using a smartphone-based device.

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Area of Science:

  • Materials Science
  • Nanotechnology
  • Environmental Chemistry

Background:

  • Single-atom nanozymes offer potential as alternatives to natural metalloenzymes but require precise structural control for optimal performance.
  • Current challenges in nanozyme design include limitations in engineering active sites for efficient catalytic activity.

Purpose of the Study:

  • To develop a facile strategy for producing iron single-atom nanozymes with multidimensional coordination engineering (Fe-N3B1/F).
  • To investigate the impact of fluorine (F) and boron (B) coordination on the electronic structure and catalytic activity of iron sites.
  • To establish a sensor platform for the detection of tetracycline antibiotics using the engineered nanozymes.

Main Methods:

  • Synthesis of iron single-atom nanozymes with Fe-N3B1/F coordination.
  • Theoretical calculations (e.g., DFT) and experimental characterization to analyze the electronic structure and reaction mechanisms.
  • Fabrication of a cross-reactive sensor array integrated with machine learning algorithms.
  • Development of a smartphone-based paper analytical device for on-site detection.

Main Results:

  • The Fe-N3B1/F nanozymes exhibited significantly enhanced peroxidase-like activity due to modulated coordination environments, overcoming limitations of traditional Fe-N4 sites.
  • The sensor array achieved intelligent pattern recognition of four homologous tetracycline antibiotics with approximately 80% accuracy.
  • The integrated smartphone-based device enabled rapid, instrument-free quantification of tetracycline antibiotics in environmental water samples.

Conclusions:

  • Multidimensional coordination engineering is a powerful strategy for designing high-performance single-atom nanozymes.
  • The developed sensor platform demonstrates a multifunctional approach for environmental monitoring of antibiotic residues.
  • This work paves the way for advanced, portable analytical devices for real-world applications.