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Insights on Dual-Functional Ionic Liquid Interfacial Layer for Efficient CO2 Electroreduction to C2+ Products in Acid
Aofei Cheng1, Jiaqi Feng1, Jiaxin Cheng1
1China University of Petroleum, Beijing, College of Chemical Engineering and Environment, National Key Laboratory of Heavy Oil, Beijing Key Laboratory of Carbon Capture and Utilization, Beijing, China.
Abstract:
Electrocatalytic CO2 reduction reaction (CO2RR) in acidic electrolyte is hindered by severe hydrogen evolution reaction (HER) and inefficient C-C coupling, leading to poor selectivity toward multicarbon (C2+) products. Here, we construct a dual-functional interfacial layer by modifying a CuO catalyst with the ionic liquid choline triazole ([Cho][Triz]). This interfacial layer simultaneously regulates the active hydrogen (*H) supply pathway to suppress HER and stabilizes key C-C coupling intermediates, thereby promoting C2+ product formation. Comprehensive in situ spectroscopic characterizations and theoretical simulations reveal that the ionic liquid interfacial layer disrupts the continuous hydrogen-bond network of interfacial water, suppresses hydronium (H3O+) transport from the bulk electrolyte, and accelerates water dissociation to generate *H species, thereby promoting intermediate hydrogenation and inhibiting HER. Meanwhile, the hydroxyl groups in the ionic liquid stabilize the *CHO intermediate and facilitate the energetically favorable asymmetric *CHO-*CO coupling pathway. Benefiting from this dual-functional regulation, the [Cho][Triz]-modified CuO catalyst delivers a C2+ Faradaic efficiency of 81.1% at 800 mA cm-2 in 1 M KCl/0.05 M H2SO4 electrolyte. Notably, the Faradaic efficiency of ethanol is approximately 2.2 times higher than that of CuO.
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