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Bioinspired Engineering of Programmable Proton-Coupled Electron Transfer in Gold Nanoclusters.

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Researchers engineered red-emissive gold nanoclusters (NCs) to mimic proton-coupled electron transfer (PCET) in enzymes. This bioinspired approach significantly enhanced electron transfer rates and sensitivity for detecting mitomycin C, advancing fluorescence sensing technologies.

Keywords:
bioinspired engineeringchitosanfluorescent probemetal nanoclusterproton-coupled electron transfer

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Area of Science:

  • Bioinspired Materials Science
  • Fluorescence Spectroscopy
  • Nanotechnology

Background:

  • Electron transfer (ET) in fluorescent probes is crucial for sensing.
  • Current ET-based probes have limitations in programmability and reaction speed.
  • Redox enzymes utilize proton-coupled electron transfer (PCET) for efficient biological reactions.

Purpose of the Study:

  • To engineer the ET pathway in red-emissive gold nanoclusters (NCs) by mimicking PCET mechanisms.
  • To enhance the controllability and rate of ET reactions in fluorescent probes.
  • To improve sensitivity and selectivity for mitomycin C detection.

Main Methods:

  • Modification of gold nanoclusters (Au9(DTT)4) by substituting chitosan with carboxylated chitosan as a secondary ligand.
  • Investigation of the ET pathway transition from pure ET to concerted PCET.
  • Characterization of photoluminescence quenching and ET rate changes.

Main Results:

  • The ligand modification successfully transformed the ET process into a PCET process.
  • A 15-fold increase in the ET rate was observed due to reduced energy barriers.
  • Photoluminescence quenching was significant, leading to over 90-fold higher sensitivity for mitomycin C detection.
  • Improved selectivity for mitomycin C was achieved.

Conclusions:

  • The study presents a novel bioinspired strategy to enhance ET-based fluorescent probes.
  • Mimicking PCET mechanisms in gold nanoclusters overcomes limitations of conventional ET probes.
  • This approach offers valuable insights for designing next-generation bioinspired sensing technologies.