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Stabilized Cu0 -Cu1+ dual sites in a cyanamide framework for selective CO2 electroreduction to ethylene
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Stabilized Cu0 -Cu1+ dual sites in a cyanamide framework for selective CO2 electroreduction to ethylene
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Journal Article
Stabilized Cu0 -Cu1+ dual sites in a cyanamide framework for selective CO2 electroreduction to ethylene
2024
Overview
Electrochemical reduction of carbon dioxide to produce high-value ethylene is often limited by poor selectivity and yield of multi-carbon products. To address this, we propose a cyanamide-coordinated isolated copper framework with both metallic copper (Cu
0
) and charged copper (Cu
1+
) sites as an efficient electrocatalyst for the reduction of carbon dioxide to ethylene. Our
operando
electrochemical characterizations and theoretical calculations reveal that copper atoms in the Cu
δ+
NCN complex enhance carbon dioxide activation by improving surface carbon monoxide adsorption, while delocalized electrons around copper sites facilitate carbon-carbon coupling by reducing the Gibbs free energy for *CHC formation. This leads to high selectivity for ethylene production. The Cu
δ+
NCN catalyst achieves 77.7% selectivity for carbon dioxide to ethylene conversion at a partial current density of 400 milliamperes per square centimeter and demonstrates long-term stability over 80 hours in membrane electrode assembly-based electrolysers. This study provides a strategic approach for designing catalysts for the electrosynthesis of value-added chemicals from carbon dioxide.
This study reports a cyanamide-framework stabilized multivalent copper catalyst for efficient electrochemical reduction of carbon dioxide to ethylene with 77.7% selectivity at 400 mA cm
−2
, offering a rational strategy for CO
2
conversion.
