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Single-stranded DNA (ssDNA) coatings on gold nanoparticles (AuNPs) precisely control the local pH at electrocatalytic interfaces. Base-pairing interactions within ssDNA layers dictate the activity and selectivity of hydroxide ion reactions.

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Area of Science:

  • Electrochemistry
  • Nanotechnology
  • Materials Science

Background:

  • Controlling the local reaction environment at electrocatalytic interfaces is critical for optimizing electrochemical reactions.
  • Single-stranded DNA (ssDNA) with anionic phosphate backbones offers potential as a novel material for modulating these interfaces.

Purpose of the Study:

  • To investigate the use of ssDNA layers as ionomer-like coatings for nanoscale control of the interfacial pH.
  • To explore how ssDNA structure, specifically strand length and base-pairing, influences electrocatalytic activity and selectivity on gold nanoparticle (AuNP) electrocatalysts.

Main Methods:

  • Fabrication of ssDNA layers on AuNP electrocatalysts with controlled thickness and base-pairing.
  • Electrochemical characterization of hydrogen evolution and glycerol oxidation reactions.
  • Structure-activity relationship analysis, including temperature-dependent studies and modified ssDNA constructs.
  • Operando surface-enhanced Raman spectroscopy (SERS) to probe interfacial mechanisms.

Main Results:

  • ssDNA layers effectively modulated the local pH and interfacial environment at the nanoscale.
  • Electrocatalytic activity and selectivity for hydroxide ion (OH-) involving reactions were dependent on the ssDNA sequence and base-pairing.
  • Base-pairing interactions within the ssDNA layer were identified as the primary factor governing catalytic performance.
  • Operando SERS revealed an ssDNA-mediated Donnan exclusion mechanism for OH-.

Conclusions:

  • ssDNA serves as a programmable platform for engineering nanoscale reaction environments in electrocatalysis.
  • Design principles for ionomer-like architectures based on ssDNA can be developed for advanced electrocatalytic applications.
  • The findings highlight the potential of DNA nanotechnology in controlling interfacial phenomena for catalysis.