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Journal of The Electrochemical Society, 2020 167 133504 Figure 2. Membrane arrangements for electrodialysis: (a) CEM-BPM, (b) AEM-BPM, (c) CEM-AEM-BPM, and (d) AEM-CEM. performed experiments using a potassium hydroxide solution in a packed column, in which sulphuric acid was used to recover the CO2, and the solution was subsequently treated using BPMs and CEMs (see Fig. 2a). Total energy demand for such a process of removing CO2 from air was estimated to be 427 kJ mol−1 CO2. Stucki et al.32 developed a similar method of atmospheric CO2 capture using a potassium hydroxide solution in a microporous membrane and subsequent Nafion-based electrodialysis membrane stack. The system also generated O2 and H2 through the electrolysis of water, with H2 exiting in the CO2 stream. Notable findings included that average cell voltage of the system for a constant current density of 100mA cm−2 had a linear dependence on potassium bicarbonate anolyte concentration for concentrations above 0.2 mol l−1, and that efficiencies for the regeneration step generally favored more open electrode structures due to enhanced mass transfer. Eisaman et al. performed BPM electrodialysis studies to inves- tigate the ability of aqueous (bi)-carbonate solutions to separate CO2 at near-atmospheric17 and elevated pressures.18 The system em- ployed AEMs to transport (bi)-carbonate from the basic chamber to the acidic chamber and BPMs to split water and provide protons (see Fig. 2b). Various mixtures of potassium (bi)-carbonate and potas- sium hydroxide solution were evaluated in terms of CO2 gas generation rate, efficiency, voltage, and energy consumption.17 Results indicated an energy consumption as low as 100 kJ mol−1 CO2 and 200kJ mol−1 CO2 to regenerate captured CO2 from aqueous bicarbonate and carbonate solutions, respectively. Current densities in the study were limited to 100 mA cm−2 due to difficulties reaching steady state at higher values. Authors performed a follow-up study with a BPM electrodialysis system working at pressures of 10 atm.18 As a result, they were able to achieve higher current densities of 139mA cm−2 and reductions in energy consumption of 29%. They also determined that the improvement in performance outweighs the additional energy costs from pressur- ization. Taniguchi et al.33 proposed a similar method of electrodialytic CO2 capture using CEMs and AEMs to treat a potassium bicarbonate solution (see Fig. 2d), but instead proposed vacuum desorption for the CO2 recovery step, resulting in theoretically lower energy requirements compared to thermal regeneration. Preliminary ther- modynamic calculations were performed showing a potential minimum work of 83 kJ mol−1 CO2 at a pressure of 6 mbar using commercial membranes. This value, authors claim, could be pushed even lower through the use of membranes with improved ion conductivity, but no bench-scale experimental work was performed. Wang et al.24 investigated a membrane electrodialysis and electrolysis setup with a single CEM and AEM to capture atmo- spheric CO2. Potassium hydroxide was electrochemically generated from O2 and H2O reduction to form hydroxide ions at the cathode (see Fig. 3a). CO2 was then recovered from the solution by reacting the potassium (bi)-carbonate with electrochemically generated sulfuric acid from protons formed at the anode through the oxygen evolution reaction. Using current densities of 2.0 mA cm−2 and cellPDF Image | CO2 Separation and Transport via Electrochemical Methods
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