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

Kaihang Yue, Yanyang Qin, Honghao Huang, Zhuoran Lv, Mingzhi Cai, Yaqiong Su (), Fuqiang Huang () and Ya Yan ()
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Kaihang Yue: Chinese Academy of Sciences
Yanyang Qin: Xi’an Jiaotong University
Honghao Huang: Chinese Academy of Sciences
Zhuoran Lv: Chinese Academy of Sciences
Mingzhi Cai: Shanghai Jiao Tong University
Yaqiong Su: Xi’an Jiaotong University
Fuqiang Huang: Chinese Academy of Sciences
Ya Yan: Chinese Academy of Sciences

Nature Communications, 2024, vol. 15, issue 1, 1-12

Abstract: 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.

Date: 2024
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DOI: 10.1038/s41467-024-52022-0

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