Enhancing CO₂ Methanation by Constructing Tetra-Atomic Catalysts on Graphdiyne.

Area of Science:

• Materials Science
• Catalysis
• Computational Chemistry

Background:

• Graphdiyne (GDY) is a 2D material with unique porous structures.
• Current research on GDY catalysts often uses single- or dual-metal configurations.
• CO2 reduction reactions (CRR) require efficient and selective catalysts.

Purpose of the Study:

• Investigate the stability and catalytic activity of tetrametallic graphdiyne (4M-GDY) systems.
• Explore the potential of 4M-GDY for CO2 reduction reactions (CRR).
• Identify descriptors for predicting catalyst selectivity in 4M-GDY systems.

Main Methods:

• Density Functional Theory (DFT) calculations were employed.
• Systematic investigation of 4M-GDY stability and catalytic activity for M = Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn.
• Analysis of magnetic moments to correlate with CRR product selectivity.

Main Results:

• 4M-GDY systems demonstrated significant deep reduction propensity.
• 4Co-GDY exhibited excellent performance for CO2 to methane (CH4) conversion, with a limiting potential of -0.46 V.
• Magnetic moment was identified as an effective descriptor for CRR product selectivity in 4M-GDY catalysts.

Conclusions:

• Tetrametallic configurations in GDY offer a platform for electronic structure modulation.
• Metal composition engineering in 4M-GDY enables rational design of efficient electrocatalysts.
• This work provides a theoretical basis for developing tailored multimetallic GDY-based catalysts for selective methane generation.