Near-unity CO₂-to-ethylene photoconversion over low coordination single-atom catalysts

Area of Science:

• Materials Science
• Catalysis
• Green Chemistry

Background:

• Photocatalytic conversion of carbon dioxide (CO₂) to chemicals is key for carbon neutrality.
• Challenges include low efficiency, selectivity, and C-C coupling due to unstable intermediates.

Purpose of the Study:

• To develop a catalyst for efficient and selective CO₂ conversion to multi-carbon products (C₂₊).
• To investigate the role of atomic-level coordination engineering in enhancing photocatalysis.

Main Methods:

• Synthesis of a low-coordination manganese single-atom catalyst embedded in zinc sulfide (Mn₁-ZnSᵥ).
• In-situ spectroscopic analyses and density functional theory (DFT) calculations.
• Evaluation of photocatalytic CO₂ conversion activity and selectivity.

Main Results:

• Mn₁-ZnSᵥ exhibits sulfur vacancies, creating a coordination-unsaturated Mn-S₂ configuration.
• The catalyst enhances CO adsorption and promotes CO/CHO coupling to *COCHO intermediates.
• Achieved 99.1% selectivity for ethylene with a formation rate of 76.6 μmol g⁻¹ h⁻¹.

Conclusions:

• Atomic-level coordination engineering of single-atom catalysts is crucial for efficient CO₂ conversion.
• The Mn₁-ZnSᵥ catalyst demonstrates a promising pathway for producing valuable chemicals from CO₂.
• This work advances the field of photocatalytic CO₂ reduction to C₂₊ products.