Ampere-level CO2 electroreduction to multi-carbon oxygenates in acidic electrolyte through surface microenvironment
Yaoyu Yin1,2, Zhongnan Ling1, Shiqiang Liu1
1Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Centre for Excellence in Molecular Sciences, Centre for Carbon Neutral Chemistry, Institute of Chemistry, Chinese Academy of Sciences, Beijing, China.
Abstract:
Efficient CO2 electroreduction to multi-carbon (C2+) oxygenates in acidic electrolytes remains a great challenge, especially under high current density conditions. In this study, we prepare an ionic liquid (IL)-modified Cu electrode (IL@Cu), which achieve a Faradaic efficiency (FE) of 82.7% toward C2+ products at a current density of 2.0 A cm-2 in 0.5 M K2SO4 (pH = 1, adjusted with H2SO4), with a single-pass carbon efficiency reaching 78.5%. Under the same conditions, the partial current density for C2+ oxygenates and ethanol exceed 1.2 A cm-2 and 1.0 A cm-2, respectively, over IL@Cu. Mechanism study has shown that K+ cations are repelled by the IL cations during the reaction, allowing water molecules to access the electrode surface. The displacement of K+ enhances C-C coupling, while the proximity of water to the electrode surface facilitates the incorporation of oxygen-containing intermediates into the hydrogen bond network, thereby promoting the formation of C2+ oxygenates.
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