Bifunctional Ionic Deep Eutectic Electrolytes for CO2 Electroreduction

Halilu, Ahmed and Hadj-Kali, Mohamed Kamel and Hashim, Mohd Ali and Yusoff, Rozita and Aroua, Mohamed Kheireddine (2022) Bifunctional Ionic Deep Eutectic Electrolytes for CO2 Electroreduction. ACS Omega, 7 (42). pp. 37764-37773. ISSN 2470-1343, DOI https://doi.org/10.1021/acsomega.2c04739.

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Official URL: https://doi.org/10.1021/acsomega.2c04739

Abstract

CO2 is a low-cost monomer capable of promoting industrially scalable carboxylation reactions. Sustainable activation of CO2 through electroreduction process (ECO2R) can be achieved in stable electrolyte media. This study synthesized and eutectic electrolyte (DEACl-DEA), using diethanolamine (DEA) as hydrogen bond donors (HBD) and diethyl ammonium chloride (DEACl) as hydrogen bond acceptors (HBA). The DEACl-DEA has -69.78 degrees C deep eutectic point and cathodic electrochemical stability limit of -1.7 V versus Ag/AgCl. In the DEACl-DEA (1:3) electrolyte, electroreduction of CO2 to CO2 center dot- was achieved at -1.5 V versus Ag/AgCl, recording a faradaic efficiency (FE) of 94%. After 350 s of continuous CO2 sparging, an asymptotic current response is reached, and DEACl-DEA (1:3) has an ambient CO2 capture capacity of 52.71 mol/L. However, DEACl-DEA has a low faradaic efficiency <94% and behaves like a regular amine during the CO2 electroreduction process when mole ratios of HBA-HBD are greater than 1:3. The electrochemical impedance spectroscopy (EIS) and COSMO-RS analyses confirmed that the bifunctional CO2 sorption by the DEACl-DEA (1:3) electrolyte promote the ECO2R process. According to the EIS, high CO2 coverage on the DEACl-DEA/Ag-electrode surface induces an electrochemical double layer capacitance (EDCL) of 3.15 x 10(-9) F, which is lower than the 8.76 x 10(-9) F for the ordinary DEACl-DEA/Ag-electrode. COSMO-RS analysis shows that the decrease in EDCL arises due to the interaction of CO2 non-polar sites (0.314, 0.097, and 0.779 e/nm(2)) with that of DEACl (0.013, 0.567 e/nm(2)) and DEA (0.115, 0.396 e/nm(2)). These results establish for the first time that a higher cathodic limit beyond the typical CO2 reduction potential is a criterion for using any deep eutectic electrolytes for sustainable CO2 electroreduction process.

Item Type: Article
Funders: King Saud University [RSP-2021/361]
Uncontrolled Keywords: CARBON-DIOXIDE CAPTURE; ELECTROCHEMICAL REDUCTION; SOLVENTS; EFFICIENT; LIQUID; ENERGY; ELECTRODES; FIXATION; STORAGE; SO2
Subjects: Q Science > QD Chemistry
Divisions: Faculty of Engineering > Department of Chemical Engineering
Depositing User: Ms. Juhaida Abd Rahim
Date Deposited: 15 Jul 2024 01:29
Last Modified: 15 Jul 2024 01:29
URI: http://eprints.um.edu.my/id/eprint/40390

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