Atomically Dispersed Cu Catalyst for Efficient Chemoselective Hydrogenation Reaction.

Area of Science:

• Materials Science
• Catalysis
• Nanotechnology

Background:

• Copper-based nanocatalysts show promise in selective hydrogenation.
• The exact catalytic mechanisms of these materials remain unclear.

Purpose of the Study:

• To develop a gram-scale synthesis for single copper atom catalysts integrated into graphitic carbon nitride (Cu1/CN).
• To elucidate the catalytic mechanism of hydrogenation reactions using these novel catalysts.

Main Methods:

• Gram-scale synthesis of single copper atom catalysts (Cu1/CN) using trimethylolmelamine.
• Characterization using X-ray absorption fine structure (XAFS).
• Computational analysis using density functional theory (DFT).

Main Results:

• Cu1/CN exhibited 100% selectivity, high activity (TOF = 2.9 × 10^3 h^-1), and excellent stability in hydrogenating 4-nitrostyrene.
• Hydroxymethyl groups in trimethylolmelamine facilitate the atomic dispersion of copper.
• XAFS confirmed a dominant Cu-N4 quaternary coordination within the melem ring.
• DFT calculations validated that anchored Cu sites provide an optimal chemical environment for efficient hydrogenation.

Conclusions:

• The developed Cu1/CN catalyst offers superior performance for selective hydrogenation.
• The study clarifies the catalytic mechanism, attributing high reactivity and selectivity to the specific coordination and electronic environment of the anchored copper atoms.