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Single-Atom Electrocatalysis for Hydrogen Evolution Based on the Constant Charge and Constant Potential Models.

Siyu Tan1, Yujin Ji1, Youyong Li1,2

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Constant potential simulations are crucial for accurately modeling single-atom electrocatalysts, especially for hydrogen evolution reactions (HER). This study reveals potential-dependent electron loss and provides insights for designing better catalysts.

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Area of Science:

  • Computational Chemistry
  • Materials Science
  • Electrochemistry

Background:

  • Density functional theory (DFT) calculations are widely used for electrocatalyst design.
  • Electrochemical reactions occur under constant potential, contrasting with constant charge DFT methods.
  • Understanding model differences is key for accurate single-atom electrocatalyst (SAC) research.

Purpose of the Study:

  • To investigate the impact of constant charge (CCM) versus constant potential (CPM) models on hydrogen adsorption in M-NC single-atom electrocatalysts.
  • To systematically study hydrogen adsorption on 99 different M-NC motifs.
  • To provide theoretical insights into the differential capacitance model for graphene-confined SACs in the hydrogen evolution reaction (HER).

Main Methods:

  • Benchmarked DFT calculations.
  • Grand-canonical DFT (GC-DFT) calculations under constant potential.
  • Systematic investigation of hydrogen adsorption on 99 M-NC motifs.

Main Results:

  • Initial electrode potentials for all M-NC motifs were found to be negative.
  • Systems lose electrons when electrode potentials are fixed at 0 V/SHE.
  • The quantitative difference in Gibbs free energy of hydrogen adsorption (ΔG(*H)) between CCM and CPM is proportional to the square of the total charge change before and after H adsorption.

Conclusions:

  • The adjustment of electronic occupation states explains the difference between CCM and CPM.
  • Constant potential model (CPM) is essential for accurate in silico design of electrocatalysts, particularly for HER.
  • This work highlights the importance of considering differential capacitance effects in graphene-confined SACs.