Graphdiyne-supported single-cluster electrocatalysts for highly efficient carbon dioxide reduction reaction

Area of Science:

• Materials Science
• Electrochemistry
• Computational Chemistry

Background:

• The electrochemical CO2 reduction reaction (CO2RR) is a key technology for mitigating CO2 emissions and producing sustainable fuels.
• Developing efficient and selective electrocatalysts is crucial for advancing CO2RR.

Purpose of the Study:

• To investigate the electrocatalytic performance of transition metal triatomic clusters embedded in graphdiyne (TM3@GDY) for CO2RR.
• To identify the most effective catalyst structure and understand the underlying mechanisms.

Main Methods:

• Density Functional Theory (DFT) calculations were employed to study various transition metal clusters.
• Ab initio molecular dynamics (AIMD) simulations were used to assess the thermodynamic stability of promising candidates.

Main Results:

• Cr3@GDY exhibited the highest catalytic activity with a low 0.39 eV rate-limiting step for CO2RR.
• Cr3@GDY effectively suppressed the competing hydrogen evolution reaction (HER).
• The superior performance is attributed to the synergistic interaction of three Cr atoms and optimized O-H interaction for hydrogenation.

Conclusions:

• Cr3@GDY is a highly efficient electrocatalyst for CO2RR, offering a promising route for CO2 conversion.
• The study provides insights into designing stable and active electrocatalysts for CO2 reduction under ambient conditions.