Work

Stabilized Cu0 -Cu1+ dual sites in a cyanamide framework for selective CO2 electroreduction to ethylene

Year: 2024

Type: article

Abstract: 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 (Cu0) and charged copper (Cu1+) 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 Cuδ+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 Cuδ+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 CO2 conversion.

Source: Nature Communications

DOI: 10.1038/s41467-024-52022-0