Computational High-Throughput Screening of Transition-Metal C₂N₂ Electrocatalysts for Oxygen Reduction Reactions

Area of Science:

• Materials Science
• Electrochemistry
• Computational Chemistry

Background:

• Efficient energy conversion technologies require stable and active electrocatalysts.
• Transition-metal (TM) nitrogen-doped carbon materials, particularly TM-C2N2, show promise for the electrochemical oxygen reduction reaction (ORR).
• Systematic studies on the effect of central atoms in TM-C2N2 on ORR performance are lacking.

Purpose of the Study:

• To systematically screen TM-C2N2 monolayer catalysts with different central atoms.
• To investigate the interaction patterns and catalytic mechanisms of TM-C2N2 in ORR.
• To identify novel, non-precious metal catalysts for efficient ORR.

Main Methods:

• Density Functional Theory (DFT) calculations.
• High-throughput screening of 38 candidate TM-C2N2 materials.
• Analysis of electronic structure, interaction patterns, and catalytic mechanisms.

Main Results:

• Altering the d-band center effectively mitigates excessive intermediate adsorption.
• The interaction strength between intermediates and TM-C2N2 dictates ORR catalytic activity.
• Ti-C2N2 and Mn-C2N2 identified as promising candidates with low overpotentials (0.34 V and 0.41 V, respectively) and high stability.

Conclusions:

• Ti-C2N2 and Mn-C2N2 are effective non-precious metal electrocatalysts for ORR.
• The d-band center and intermediate interaction strength are key factors for ORR performance in TM-C2N2.
• This research provides theoretical guidance for designing advanced ORR catalysts.