Engineering Atom-Scale Cascade Catalysis via Multi-Active Site Collaboration for Ampere-Level CO₂ Electroreduction to...

Area of Science:

• Electrochemistry
• Materials Science
• Catalysis

Background:

• Electrochemical reduction of CO2 to multicarbon products is key for energy storage and CO2 utilization.
• Achieving high C2+ selectivity at industrial current densities remains a significant challenge.

Purpose of the Study:

• To develop a catalyst for efficient electrochemical reduction of CO2 to C2+ products.
• To investigate the catalytic mechanism at the atomic level.

Main Methods:

• Synthesis of a Mo1Cu single-atom alloy (SAA) catalyst.
• Electrochemical performance testing under high current density.
• Operando spectroscopy and density functional theory (DFT) calculations.

Main Results:

• Mo1Cu SAA catalyst achieved 86.4% C2+ Faradaic efficiency at 0.80 A cm-2.
• Reached a C2+ partial current density of 1.33 A cm-2 with >74.3% Faradaic efficiency.
• Operando spectroscopy and DFT revealed atom-scale cascade catalysis via synergistic Mo and Cu sites.

Conclusions:

• The Mo1Cu SAA catalyst facilitates CO2 activation and C-C coupling through multi-active site collaboration.
• Mo sites promote H2O dissociation, while Cu sites activate CO2 and facilitate CO coupling.
• This work provides insights for designing advanced tandem electrocatalysts for CO2 conversion to multicarbon products.