Cation Solvation Engineering for enhanced CO2 Electroreduction

Haoran Zhang

doi:10.1039/D5SE01163A

Cation Solvation Engineering for enhanced CO2 Electroreduction

2025-10-10

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Tribidasari A. Ivandini

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Sheng Zhang

DOI：10.1039/D5SE01163A

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Electrochemical CO 2 reduction (CO 2 RR) holds promise for carbon-neutral fuel production but is hindered by the competing hydrogen evolution reaction (HER) and slow kinetics. This study investigates how cationic solvation engineering with 18crown-6 ether (18C6) impacts CO 2 RR by selectively coordinating potassium ions (K + ).18C6 disrupts the K + hydration shell; shifting the proton source from water to bicarbonate; suppressing HER; and enhancing CO 2 RR. Experimental results show a 7.3-fold increase in CO Faradaic efficiency (FE) with optimized 18C6 concentrations in 1 M KHCO 3 . The non-monotonic relationship between CO production rates and 18C6 concentration highlights the balance between water and bicarbonate protonation processes. In-situ ATR-FTIR and Raman analyses reveal reduced water adsorption and enhanced carbonate interactions at the electrode interface. Temperature-dependent electrochemical impedance spectroscopy demonstrates a lowered desolvation energy barrier (83.4 vs. 32.1 kJ mol -1 ); indicating facilitated dehydration of solvated K + . This work provides insights into the mechanistic role of cationic solvation; offering a strategy for improving CO 2 RR efficiency.

Cation Solvation Engineering for enhanced CO2 Electroreduction

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