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Stabilizing Cu+ Sites at Cu2O(111)-ZrO2 Heterointerfaces for Durable and Selective CO2-to-C2H4 Electroreduction
Yuning Lou1, Yuejiang Han1, Yuxuan Zhang1
1College of Chemistry, Liaoning University, Shenyang110036, P. R. China.
Engineered Cu2O-ZrO2 heterointerfaces stabilize key copper species, significantly boosting ethylene production from CO2 electroreduction (CO2RR) with enhanced selectivity and durability.
Area of Science:
- Materials Science
- Electrochemistry
- Catalysis
Background:
- Copper oxide (Cu2O) is promising for CO2 electroreduction (CO2RR) but struggles with ethylene selectivity.
- Insufficient stabilization of Cu+ limits C-C coupling and catalyst durability.
Purpose of the Study:
- To engineer Cu2O(111)-ZrO2 heterointerfaces for improved CO2RR.
- To enhance Cu+ stabilization and promote C-C coupling for ethylene production.
Main Methods:
- Fabrication of Cu2O-ZrO2 interfaces within a carbon matrix (CuZr@C) using a metal-organic framework template.
- Electrochemical evaluation in H and flow cells.
- Operando X-ray absorption spectroscopy and Raman spectroscopy.
- Density functional theory (DFT) calculations.
Main Results:
- CuZr@C achieved 72.1% Faradaic efficiency for ethylene (FEC2H4) at 39.0 mA cm-2 with excellent durability (>70% retention over 120 h).
- Operando studies confirmed Cu+ stabilization and high CO coverage at the interface.
- DFT revealed a reduced activation barrier for the key C-C coupling step (0.68 eV).
Conclusions:
- Nanoscale Cu2O-ZrO2 heterointerfaces effectively stabilize Cu+ and promote CO2RR to ethylene.
- This strategy offers a viable pathway for developing durable and selective catalysts for multicarbon product synthesis.
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