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Elementary kinetics of nitrogen electroreduction on Fe surfaces.

Sharad Maheshwari1, Gholamreza Rostamikia2, Michael J Janik1

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Electrochemical ammonia synthesis offers a sustainable alternative to the Haber-Bosch process. DFT calculations reveal interfacial water and cathodic potentials below -1.5 V-RHE are crucial for efficient nitrogen electroreduction on Fe surfaces.

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Area of Science:

  • Electrochemistry
  • Materials Science
  • Computational Chemistry

Background:

  • The Haber-Bosch process is energy-intensive.
  • Electrochemical ammonia synthesis is a sustainable alternative.
  • Catalyst design requires mechanistic understanding.

Purpose of the Study:

  • Investigate nitrogen electroreduction mechanisms on Fe surfaces.
  • Determine elementary step energetics using DFT.
  • Connect catalyst properties to performance.

Main Methods:

  • Density Functional Theory (DFT) calculations.
  • Analysis of associative N2 reduction mechanisms.
  • Examination of elementary step energetics on Fe surfaces.

Main Results:

  • Interfacial water molecules lower activation barriers in the Heyrovsky-like mechanism.
  • Cathodic potentials below -1.5 V-RHE are needed for significant N2 electroreduction rates.
  • DFT barriers indicate a larger overpotential than predicted by free energies.

Conclusions:

  • Explicit barrier calculations are essential for DFT studies of nitrogen reduction.
  • Brønsted-Evans-Polanyi relationships do not universally apply to N-H formation steps.
  • Understanding reaction mechanisms is key to designing efficient electrocatalysts.