Conversion of methane to C₂ liquid oxygenates by Ru atom arrays

Area of Science:

• Catalysis
• Materials Science
• Chemical Engineering

Background:

• Efficient conversion of methane to value-added chemicals remains a significant challenge.
• Developing selective catalysts for C-C coupling is crucial for C2 oxygenate production.

Purpose of the Study:

• To develop a new catalytic system for selective C-C coupling of methane to C2 liquid oxygenates.
• To investigate the role of anchored ruthenium atoms on graphdiyne in methane activation and conversion.

Main Methods:

• Synthesis of a catalytic system with zero-valent ruthenium atoms anchored in a graphdiyne cavity.
• Experimental characterization of the catalytic system.
• Theoretical calculations (Density Functional Theory) to understand the reaction mechanism.

Main Results:

• Selective anchoring of individual to три-atom ruthenium clusters (Ru-GDY) within graphdiyne.
• Ru3-GDY demonstrated neighboring robust active sites promoting C-C coupling.
• Achieved high selectivity (67%) and yield (7.25 mmol gcat−1 h−1) towards C2 liquid oxygenates.
• Identified p-d coupling resonance as key to distributed charge and accelerated methane oxidation.

Conclusions:

• The Ru-GDY catalytic system enables highly efficient and selective methane activation to key intermediates.
• This facilitates selective C-C coupling for C2 liquid oxygenate production.
• The findings offer a promising pathway for methane valorization.