Insight into the role of imidazolium cations in regulating Ag electrode interface for enhancing electrochemical CO2 reduction

doi:10.1016/S1872-2067(25)64886-8

Abstract

Abstract:

Imidazolium-based ionic liquids (ILs) exhibit great potential in promoting electrochemical CO₂ reduction reaction (CO₂RR) by reducing overpotential reduction and enhancing catalytic efficiency. However, the regulatory role of ILs structure in the local physicochemical region at the electrode/electrolyte interface and in reaction kinetics remain unclear. In this study, we designed imidazolium-based ILs with tunable cation alkyl chain length and systematically revealed the dynamic interfacial regulation mechanism controlled by cation structure, based on in-situ infrared spectroscopy and molecular dynamics simulations. The commercial Ag electrodes in electrolytes with critical chain length exhibit nearly 100% Faradaic efficiency for CO production while maintaining high current density. Imidazolium cations with critical chain length effectively regulate the electric double layer at the Ag electrode/electrolyte interface: they notably balance a range of positive and negative factors, including hydrophobicity, CO₂ absorption, conductivity, viscosity, and hydrogen evolution reaction, etc. Collectively, these effects synergistically shape an optimized interfacial local physicochemical region, enhancing the rate of CO₂ catalytic reactions. This work elucidates the mechanistic framework of interfacial regulation in CO₂RR and delivers molecular design principles for engineering IL-based electrolytes toward enhanced catalytic selectivity.

Key words: Ionic liquids, Cation alkyl chain length, CO₂ reduction reaction, Molecular dynamics simulations, Electrolyte

Diankun Song, Yunyun Wu, Jiahui Hua, Chunfeng Shao, Zhaoyang Wei, Jianji Wang, Kai Dai. Insight into the role of imidazolium cations in regulating Ag electrode interface for enhancing electrochemical CO₂ reduction[J]. Chinese Journal of Catalysis, 2026, 81: 206-215.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(25)64886-8

https://www.cjcatal.com/EN/Y2026/V81/I2/206

Figures/Tables 5

Fig. 1. (a) Contact angles at the Ag electrodes and electrolyte interfaces. (b) CO2 absorption capacities at a flow rate of 10 mL min?1.

Fig. 2. Electrochemical performance of five different electrolytes on the Ag electrodes. (a) LSV curves under CO2 saturation. (b) Tafel plots. (c) FECO at five potentials. (d) JCO at five potentials.

Fig. 3. (a) In-situ ATR-SEIRAS spectra of E(iii) on the Ag electrodes, along with the amplified spectra of its C-H vibration peaks (b). (c) Structure of C8Mim+.

Fig. 4. (a) Typical snapshots of the three electrolytes under non-working and working conditions. The NDD curves (b) and MSD curves (c) of the three electrolytes under non-working conditions, and the NDD curves (d) and MSD curves (e) under working conditions.

Fig. 5. The CO2 transport ability from the end of the alkyl chain of the ionic liquid to the electrodes interface, the model illustrated here corresponds to the E(iii).

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Insight into the role of imidazolium cations in regulating Ag electrode interface for enhancing electrochemical CO₂ reduction

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