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Jin, Shijian

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Jin

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Shijian

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Jin, Shijian

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  • Publication
    pH swing cycle for CO2 capture electrochemically driven through proton-coupled electron transfer
    (Royal Society of Chemistry (RSC), 2020) Jin, Shijian; Wu, Min; Gordon, Roy; Aziz, Michael; Kwabi, David
    We perform a thermodynamic analysis of the energetic cost of CO2 separation from flue gas (0.1 bar CO2(g)) and air (400 ppm CO2) using a pH swing created by electrochemical redox reactions involving proton-coupled electron transfer from molecular species in aqueous electrolyte. In this scheme, electrochemical reduction of these molecules results in the formation of alkaline solution, into which CO2 is absorbed; subsequent electrochemical oxidation of the reduced molecules results in the acidification of the solution, triggering the release of pure CO2 gas. We examined the effect of buffering from the CO2–carbonate system on the solution pH during the cycle, and thereby on the open-circuit potential of an electrochemical cell in an idealized four-process CO2 capture-release cycle. The minimum work input varies from 16 to 75 kJ molCO2−1 as throughput increases, for both flue gas and direct air capture, with the potential to go substantially lower if CO2 capture or release is performed simultaneously with electrochemical reduction or oxidation. We discuss the properties required of molecules that would be suitable for such a cycle. We also demonstrate multiple experimental cycles of an electrochemical CO2 capture and release system using 0.078 M sodium 3,3′-(phenazine-2,3-diylbis(oxy))bis(propane-1-sulfonate) as the proton carrier in an aqueous flow cell. CO2 capture and release are both performed at 0.465 bar at a variety of current densities. When extrapolated to infinitesimal current density we obtain an experimental cycle work of 47.0 kJ molCO2−1. This result suggests that, in the presence of a 0.465 bar/1.0 bar inlet/outlet pressure ratio, a 1.9 kJ molCO2−1 thermodynamic penalty should add to the measured value, yielding an energy cost of 48.9 kJ molCO2−1 in the low-current-density limit. This result is within a factor of two of the ideal cycle work of 34 kJ molCO2−1 for capturing at 0.465 bar and releasing at 1.0 bar. The ideal cycle work and experimental cycle work values are compared with those for other electrochemical and thermal CO2 separation methods.
  • Publication
    Low Energy Carbon Capture via Electrochemically Induced pH Swing with Electrochemical Rebalancing
    (Cambridge University Press (CUP), 2021-09-13) Jin, Shijian; Wu, Min; Jing, Yan; Gordon, Roy; Aziz, Michael
    We demonstrate a carbon capture system based on pH swing cycles driven through proton-coupled electron transfer of sodium (3,3’-(phenazine-2,3-diylbis(oxy))bis(propane-1-sulfonate)) (DSPZ) molecules. Electrochemical reduction of DSPZ causes an increase of hydroxide concentration, which absorbs CO2; subsequent electrochemical oxidation of the reduced DSPZ consumes the hydroxide, causing CO2 outgassing. The measured electrical work of separating CO2 from a binary mixture with N2, at CO2 inlet partial pressures ranging from 0.1 to 0.5 bar, and releasing to a pure CO2 exit stream at 1.0 bar, was measured for electrical current densities of 20 to 150 mA/ cm2. The work for separating CO2 from a 0.1 bar inlet and concentrating into 1 bar exit is 61.3 kJ/molCO2 at a current density of 20 mA/cm2 and extrapolates to 57.1 kJ/molCO2 in the low-current-density limit. At this limit, the cycle work for capture from 0.4 mbar extrapolates to 108-212 kJ/ molCO2 depending on the initial composition of the electrolyte. We also introduce an electrochemical rebalancing method that extends cell lifetime by recovering the initial electrolyte composition after it is perturbed by side reactions. We discuss the implications of these results for future low-energy electrochemical carbon capture devices.