Br, O-Modified Cu(111) Interface Promotes CO₂ Reduction to Multicarbon Products.

Area of Science:

• Electrochemistry
• Materials Science
• Catalysis

Background:

• Electrochemical reduction of CO₂ (CO₂RR) to C₂₊ products is key for a carbon-neutral economy.
• Controlling catalytic selectivity at the interface is crucial for efficient C₂₊ production.

Purpose of the Study:

• To design and investigate a novel Cu/UIO-Br interface for enhanced CO₂ electroreduction.
• To elucidate the catalytic mechanism for selective C₂₊ product formation.

Main Methods:

• Fabrication of a Cu/UIO-Br interface with simultaneous Br and O co-modification.
• Electrochemical performance evaluation using an H-cell electrolyzer.
• Mechanistic studies including kinetic isotopic effect, in situ ATR-FTIR, and DFT calculations.

Main Results:

• The Cu/UIO-Br interface achieved a ≈53% Faradaic efficiency for C₂₊ products (ethanol/ethylene).
• A high C₂₊ partial current density of 24.3 mA cm^-2 was recorded.
• Co-modification enhanced CO₂ adsorption and promoted the formation of key intermediates via hydrogen-bonding effects.

Conclusions:

• The Br, O co-modified Cu(111) interface effectively promotes C₂₊ selectivity in CO₂ electroreduction.
• Understanding the catalytic mechanism involving hydrogen-bonding and intermediate coupling is vital.
• This strategy provides a pathway for designing advanced Cu-based catalysts for C₂₊ production.