Stabilized Cu<sup>0</sup> -Cu<sup>1+</sup> dual sites in a cyanamide framework for selective CO<sub>2</sub> electroreduction to ethylene.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 39242556.
- Also identified by DOI 10.1038/s41467-024-52022-0 and PMC identifier 11379946.
- Licence recorded as CC BY-NC-ND.
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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 (Cu<sup>0</sup>) and charged copper (Cu<sup>1+</sup>) 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<sup>δ+</sup>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<sup>δ+</sup>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.