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Electrochemical regeneration of high-purity CO2 from (bi)carbonates in a porous solid electrolyte reactor for efficient carbon capture

Abstract

Carbon dioxide (CO2) and absorbent regeneration are the most energy-intensive processes in carbon capture loops. Conventional carbon capture technologies typically consume substantial amounts of heat and involve multiple steps for regeneration. Here we demonstrated one-step electrochemical regeneration of CO2 and alkaline absorbent from carbon-containing solutions in a modular porous solid electrolyte (PSE) reactor. By performing hydrogen evolution and oxidation redox reactions, our PSE reactor selectively split NaHCO3/Na2CO3 solutions, which typically come from air contactors after CO2 absorption, into NaOH absorbent in the catholyte and high-purity CO2 gas in the PSE layer. No chemicals were consumed and no by-products were generated. High Na+-ion transport number (~90%), high capture capacity retention (~90%), low energy consumptions (50 kJ molCO2−1 and 118 kJ molCO2−1 at 1 mA cm−2 and 100 mA cm−2 for bicarbonate, respectively) and long-term stability (>100 hours) were demonstrated. We achieved industrially relevant carbon regeneration rates of up to 1 A cm−2 (~18 mmol cm−2 h−1), highlighting the promising application potential.

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Fig. 1: Comparison between thermal and electrochemical CO2 regeneration in the CO2–carbonate carbon capture loop.
Fig. 2: Comparison between our porous solid electrolyte reactor design and traditional electrolysers for CO2 regeneration from (bi)carbonates.
Fig. 3: The CO2 regeneration performance under a continuous flow of NaHCO3 and Na2CO3 solutions through the middle PSE layer with different concentrations.
Fig. 4: Carbon balance analysis in a electrolyte recirculation mode.
Fig. 5: Practical cycle operations for CO2 regeneration in our PSE reactor.

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Data availability

The data supporting the findings of this study are available in the main text, Supplementary Information and source data provided with this paper. Additional data related to this study may be requested from the corresponding author. Source data are provided with this paper.

References

  1. Chu, S. Carbon capture and sequestration. Science 325, 1599 (2009).

    MATH  Google Scholar 

  2. Goeppert, A., Czaun, M., Prakash, G. S. & Olah, G. A. Air as the renewable carbon source of the future: an overview of CO2 capture from the atmosphere. Energy Environ. Sci. 5, 7833–7853 (2012).

    Google Scholar 

  3. Keith, D. W., Holmes, G., Angelo, D. S. & Heidel, K. A process for capturing CO2 from the atmosphere. Joule 2, 1573–1594 (2018).

    MATH  Google Scholar 

  4. Buckingham, J., Reina, T. R. & Duyar, M. S. Recent advances in carbon dioxide capture for process intensification. Carbon Capture Sci. Technol. 2, 100031 (2022).

    MATH  Google Scholar 

  5. Sanz-Pérez, E. S., Murdock, C. R., Didas, S. A. & Jones, C. W. Direct capture of CO2 from ambient air. Chem. Rev. 116, 11840–11876 (2016).

    Google Scholar 

  6. Rochelle, G. T. Amine scrubbing for CO2 capture. Science 325, 1652–1654 (2009).

    MATH  Google Scholar 

  7. Voskian, S. & Hatton, T. A. Faradaic electro-swing reactive adsorption for CO2 capture. Energy Environ. Sci. 12, 3530–3547 (2019).

    MATH  Google Scholar 

  8. Eisaman, M. D. et al. CO2 extraction from seawater using bipolar membrane electrodialysis. Energy Environ. Sci. 5, 7346–7352 (2012).

    Google Scholar 

  9. Zhu, P. et al. Continuous carbon capture in an electrochemical solid-electrolyte reactor. Nature 618, 959–966 (2023).

    MATH  Google Scholar 

  10. Shu, Q., Legrand, L., Kuntke, P., Tedesco, M. & Hamelers, H. V. Electrochemical regeneration of spent alkaline absorbent from direct air capture. Environ. Sci. Technol. 54, 8990–8998 (2020).

    Google Scholar 

  11. Liu, J. et al. Hydrogen-motivated electrolysis of sodium carbonate with extremely low cell voltage. Chem. Commun. 54, 3582–3585 (2018).

    MATH  Google Scholar 

  12. Muroyama, A. P. & Gubler, L. Carbonate regeneration using a membrane electrochemical cell for efficient CO2 capture. ACS Sustain. Chem. Eng. 10, 16113–16117 (2022).

    Google Scholar 

  13. Bougie, F. & Fan, X. Microwave regeneration of monoethanolamine aqueous solutions used for CO2 capture. Int. J. Greenh. Gas. Control 79, 165–172 (2018).

    MATH  Google Scholar 

  14. Bougie, F. & Iliuta, M. C. Analysis of regeneration of sterically hindered alkanolamines aqueous solutions with and without activator. Chem. Eng. Sci. 65, 4746–4750 (2010).

    MATH  Google Scholar 

  15. Yoo, M., Han, S.-J. & Wee, J.-H. Carbon dioxide capture capacity of sodium hydroxide aqueous solution. J. Environ. Manag. 114, 512–519 (2013).

    MATH  Google Scholar 

  16. Halliday, C. & Hatton, T. A. Sorbents for the capture of CO2 and other acid gases: a review. Ind. Eng. Chem. Res. 60, 9313–9346 (2021).

    MATH  Google Scholar 

  17. Stolaroff, J. K., Keith, D. W. & Lowry, G. V. Carbon dioxide capture from atmospheric air using sodium hydroxide spray. Environ. Sci. Technol. 42, 2728–2735 (2008).

    Google Scholar 

  18. Watkins, J. D. et al. Redox-mediated separation of carbon dioxide from flue gas. Energy Fuels 29, 7508–7515 (2015).

    MATH  Google Scholar 

  19. Renfrew, S. E., Starr, D. E. & Strasser, P. Electrochemical approaches toward CO2 capture and concentration. ACS Catal. 10, 13058–13074 (2020).

    Google Scholar 

  20. Rheinhardt, J. H., Singh, P., Tarakeshwar, P. & Buttry, D. A. Electrochemical capture and release of carbon dioxide. ACS Energy Lett. 2, 454–461 (2017).

    Google Scholar 

  21. Eisaman, M. D., Alvarado, L., Larner, D., Wang, P. & Littau, K. A. CO2 desorption using high-pressure bipolar membrane electrodialysis. Energy Environ. Sci. 4, 4031–4037 (2011).

    Google Scholar 

  22. Sharifian, R., Wagterveld, R., Digdaya, I., Xiang, C.-X. & Vermaas, D. Electrochemical carbon dioxide capture to close the carbon cycle. Energy Environ. Sci. 14, 781–814 (2021).

    Google Scholar 

  23. Willauer, H. D., DiMascio, F., Hardy, D. R. & Williams, F. W. Development of an electrolytic cation exchange module for the simultaneous extraction of carbon dioxide and hydrogen gas from natural seawater. Energy Fuels 31, 1723–1730 (2017).

    MATH  Google Scholar 

  24. Gurkan, B. et al. Perspective and challenges in electrochemical approaches for reactive CO2 separations. iScience 24, 103422 (2021).

    MATH  Google Scholar 

  25. Xia, R., Overa, S. & Jiao, F. Emerging electrochemical processes to decarbonize the chemical industry. JACS Au 2, 1054–1070 (2022).

    MATH  Google Scholar 

  26. Digdaya, I. A. et al. A direct coupled electrochemical system for capture and conversion of CO2 from oceanwater. Nat. Commun. 11, 4412 (2020).

    MATH  Google Scholar 

  27. Liu, Y., Ye, H.-Z., Diederichsen, K. M., Van Voorhis, T. & Hatton, T. A. Electrochemically mediated carbon dioxide separation with quinone chemistry in salt-concentrated aqueous media. Nat. Commun. 11, 2278 (2020).

    Google Scholar 

  28. Rau, G. H., Willauer, H. D. & Ren, Z. J. The global potential for converting renewable electricity to negative-CO2-emissions hydrogen. Nat. Clim. Change 8, 621–625 (2018).

    MATH  Google Scholar 

  29. Wang, M., Herzog, H. J. & Hatton, T. A. CO2 capture using electrochemically mediated amine regeneration. Ind. Eng. Chem. Res. 59, 7087–7096 (2020).

    Google Scholar 

  30. Welch, A. J., Dunn, E., DuChene, J. S. & Atwater, H. A. Bicarbonate or carbonate processes for coupling carbon dioxide capture and electrochemical conversion. ACS Energy Lett. 5, 940–945 (2020).

    Google Scholar 

  31. Gilliam, R. J. et al. Low voltage electrochemical process for direct carbon dioxide sequestration. J. Electrochem. Soc. 159, B627 (2012).

    MATH  Google Scholar 

  32. Park, H. S. et al. CO2 fixation by membrane separated NaCl electrolysis. Energies 8, 8704–8715 (2015).

    Google Scholar 

  33. Stucki, S., Schuler, A. & Constantinescu, M. Coupled CO2 recovery from the atmosphere and water electrolysis: feasibility of a new process for hydrogen storage. Int. J. Hydrogen Energy 20, 653–663 (1995).

    MATH  Google Scholar 

  34. Rahimi, M. et al. Carbon dioxide capture using an electrochemically driven proton concentration process. Cell Rep. Phys. Sci 1, 100033 (2020).

    MATH  Google Scholar 

  35. Prajapati, A. et al. Migration-assisted, moisture gradient process for ultrafast, continuous CO2 capture from dilute sources at ambient conditions. Energy Environ. Sci. 15, 680–692 (2022).

    MATH  Google Scholar 

  36. Legrand, L., Shu, Q., Tedesco, M., Dykstra, J. & Hamelers, H. Role of ion exchange membranes and capacitive electrodes in membrane capacitive deionization (MCDI) for CO2 capture. J. Colloid Interface Sci. 564, 478–490 (2020).

    Google Scholar 

  37. Willauer, H. D., DiMascio, F., Hardy, D. R. & Williams, F. W. Feasibility of CO2 extraction from seawater and simultaneous hydrogen gas generation using a novel and robust electrolytic cation exchange module based on continuous electrodeionization technology. Ind. Eng. Chem. Res. 53, 12192–12200 (2014).

    Google Scholar 

  38. de Lannoy, C.-F. et al. Indirect ocean capture of atmospheric CO2: part I. Prototype of a negative emissions technology. Int. J. Greenh. Gas. Control 70, 243–253 (2018).

    MATH  Google Scholar 

  39. Sharifian, R., Boer, L., Wagterveld, R. & Vermaas, D. Oceanic carbon capture through electrochemically induced in situ carbonate mineralization using bipolar membrane. Chem. Eng. J. 438, 135326 (2022).

    Google Scholar 

  40. Mehmood, A. et al. A novel high performance configuration of electrochemical cell to produce alkali for sequestration of carbon dioxide. Electrochim. Acta 219, 655–663 (2016).

    MATH  Google Scholar 

  41. Xia, C., Xia, Y., Zhu, P., Fan, L. & Wang, H. Direct electrosynthesis of pure aqueous H2O2 solutions up to 20% by weight using a solid electrolyte. Science 366, 226–231 (2019).

    MATH  Google Scholar 

  42. Xia, C. et al. Continuous production of pure liquid fuel solutions via electrocatalytic CO2 reduction using solid-electrolyte devices. Nat. Energy 4, 776–785 (2019).

    MATH  Google Scholar 

  43. Kim, J. Y. T. et al. Recovering carbon losses in CO2 electrolysis using a solid electrolyte reactor. Nat. Catal. 5, 288–299 (2022).

    MATH  Google Scholar 

  44. Shin, H., Hansen, K. U. & Jiao, F. Techno-economic assessment of low-temperature carbon dioxide electrolysis. Nat. Sustain. 4, 911–919 (2021).

    MATH  Google Scholar 

  45. FY 2018 Progress Report for the DOE Hydrogen and Fuel Cells Program (US Department of Energy, 2019).

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Acknowledgements

This work was supported by the Robert A. Welch Foundation (grant number C-2051-20230405) and the David and Lucile Packard Foundation (grant number 2020-71371).

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Contributions

X.Z. and H.W. conceived the project and designed the experiments. X.Z. and Z.F. performed the experimental study. P.Z. performed the TEA study. Y.X. performed the energy consumption comparison of different methods. X.Z. and H.W. wrote the paper with support from all authors. H.W. supervised this project.

Corresponding authors

Correspondence to Xiao Zhang or Haotian Wang.

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Competing interests

X.Z. and H.W. are listed as inventors on a patent application filed by the Rice University that pertains to this work. The other authors declare no competing interests.

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Nature Energy thanks Ung Lee and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Zhang, X., Fang, Z., Zhu, P. et al. Electrochemical regeneration of high-purity CO2 from (bi)carbonates in a porous solid electrolyte reactor for efficient carbon capture. Nat Energy 10, 55–65 (2025). https://doi.org/10.1038/s41560-024-01654-z

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