Catalyst-electrolyte Interactions in Aqueous Reline Solutions for Highly Selective Electrochemical CO2 Reduction

Garg, Sahil and Li, Mengran and Rufford, Thomas E. and Ge, Lei ORCID: https://orcid.org/0000-0003-2989-0329 and Rudolph, Victor and Knibbe, Ruth and Konarova, Muxina and Wang, Geoff G.X. (2020) Catalyst-electrolyte Interactions in Aqueous Reline Solutions for Highly Selective Electrochemical CO2 Reduction. ChemSusChem, 13 (2). pp. 304-311. ISSN 1864-5631


Abstract

Achieving high product selectivities is one challenge that limits viability of electrochemical CO2 reduction (CO2R) to chemical feedstocks. Here, it was demonstrated how interactions between Ag foil cathodes and reline (choline chloride + urea) led to highly selective CO2R to CO with a faradaic efficiency of (96±8) % in 50 wt % aqueous reline at −0.884 V vs. the reversible hydrogen electrode (RHE), which is a 1.5‐fold improvement over CO2R in KHCO3. In reline the Ag foil was roughened by (i) dissolution of oxide layers followed by (ii) electrodeposition of Ag nanoparticles back on cathode. This surface restructuring exposed low‐coordinated Ag atoms, and subsequent adsorption of choline ions and urea at the catalyst surface limited proton availability in the double layer and stabilized key intermediates such as *COOH. These approaches could potentially be extended to other electrocatalytic metals and lower‐viscosity deep eutectic solvents to achieve higher‐current‐density CO2R in continuous‐flow cell electrolyzers.


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Item Type: Article (Commonwealth Reporting Category C)
Refereed: Yes
Item Status: Live Archive
Additional Information: Files associated with this item cannot be displayed due to copyright restrictions.
Faculty/School / Institute/Centre: Current - Institute for Advanced Engineering and Space Sciences - Centre for Future Materials (1 Jan 2017 -)
Faculty/School / Institute/Centre: Current - Institute for Advanced Engineering and Space Sciences - Centre for Future Materials (1 Jan 2017 -)
Date Deposited: 16 Jun 2020 05:03
Last Modified: 27 Jul 2020 00:11
Uncontrolled Keywords: catalyst–electrolyte interactions; CO2 reduction; electrochemistry; reline; silver
Fields of Research (2008): 03 Chemical Sciences > 0302 Inorganic Chemistry > 030207 Transition Metal Chemistry
09 Engineering > 0904 Chemical Engineering > 090402 Catalytic Process Engineering
Fields of Research (2020): 34 CHEMICAL SCIENCES > 3402 Inorganic chemistry > 340211 Transition metal chemistry
40 ENGINEERING > 4004 Chemical engineering > 400408 Reaction engineering (excl. nuclear reactions)
Socio-Economic Objectives (2008): B Economic Development > 86 Manufacturing > 8606 Industrial Chemicals and Related Products > 860601 Industrial Gases
Identification Number or DOI: https://doi.org/10.1002/cssc.201902433
URI: http://eprints.usq.edu.au/id/eprint/37904

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