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- Title
Stabilized Cu<sup>0</sup> -Cu<sup>1+</sup> dual sites in a cyanamide framework for selective CO<sub>2</sub> electroreduction to ethylene.
- Authors
Yue, Kaihang; Qin, Yanyang; Huang, Honghao; Lv, Zhuoran; Cai, Mingzhi; Su, Yaqiong; Huang, Fuqiang; Yan, Ya
- 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.
- Subjects
GIBBS' free energy; ELECTRON delocalization; COPPER catalysts; COPPER; ELECTROSYNTHESIS; CARBON dioxide; ELECTROLYTIC reduction; CARBON dioxide reduction
- Publication
Nature Communications, 2024, Vol 15, Issue 1, p1
- ISSN
2041-1723
- Publication type
Article
- DOI
10.1038/s41467-024-52022-0