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Boyuan Zhang1, Cedric Schaack2, Claudia R Prindle2

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This study shows electric fields can initiate and accelerate chemical reactions in solution, like the cleavage of a radical initiator. Reaction rates correlate with solvent properties, offering new catalytic methods.

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Area of Science:

  • Chemistry
  • Physical Chemistry
  • Materials Science

Background:

  • External electric fields are challenging to apply for activating reactions in bulk solution.
  • Previous methods for electric field control of reactions were limited.

Purpose of the Study:

  • To investigate electric field-driven homolytic cleavage of a specific radical initiator.
  • To characterize the reaction kinetics and mechanism in bulk solution.

Main Methods:

  • Utilized scanning tunneling microscope-based break-junction technique.
  • Employed time-dependent ex situ quantification via high-performance liquid chromatography (HPLC) with UV-vis detection.
  • Performed density functional theory (DFT) calculations.

Main Results:

  • Demonstrated electric field catalysis of radical initiator cleavage at ambient temperatures.
  • Found reaction rate increases linearly with solvent dielectric constant.
  • Showed electric fields decrease O-O bond dissociation energy and stabilize products.

Conclusions:

  • Electric fields can effectively catalyze chemical reactions in bulk solution.
  • Solvent dielectric properties significantly influence electric field-driven reaction rates.
  • DFT calculations elucidate the mechanism of electric field-induced bond cleavage and product stabilization.