Skip to main content

Thank you for visiting nature.com. You are using a browser version with limited support for CSS. To obtain the best experience, we recommend you use a more up to date browser (or turn off compatibility mode in Internet Explorer). In the meantime, to ensure continued support, we are displaying the site without styles and JavaScript.

A shorted membrane electrochemical cell powered by hydrogen to remove CO2 from the air feed of hydroxide exchange membrane fuel cells

Abstract

The alkaline environment of hydroxide exchange membrane fuel cells (HEMFCs) potentially allows use of cost-effective catalysts and bipolar plates in devices. However, HEMFC performance is adversely affected by CO2 present in the ambient air feed. Here, we demonstrate an electrochemically driven CO2 separator (EDCS) to remove CO2 from the air feed using a shorted membrane that conducts both anions and electrons. This EDCS is powered by hydrogen like a fuel cell but needs no electrical wires, bipolar plates or current collectors, and thus can be modularized like a typical separation membrane. We show that a 25 cm2 shorted membrane EDCS can achieve >99% CO2 removal from 2,000 standard cubic centimetres per minute (sccm) of air for 450 hours and operate effectively under load-following dynamic conditions. A spiral-wound EDCS module can remove >98% CO2 from 10,000 sccm of air. Our technoeconomic analysis indicates a compact and efficient module at >99% CO2 removal costs US$112 for an 80 kWnet HEMFC stack.

This is a preview of subscription content

Access options

Buy article

Get time limited or full article access on ReadCube.

$32.00

All prices are NET prices.

Fig. 1: Effect of CO2 on HEMFC performance.
Fig. 2: Working principle of the shorted membrane EDCS.
Fig. 3: Preparation and properties of the shorted membrane.
Fig. 4: Control of the shorted membrane EDCS by hydrogen supply.
Fig. 5: Performance and durability for the shorted membrane EDCS.
Fig. 6: Demonstration of the spiral-wound EDCS module.
Fig. 7: Economic analysis for the EDCS module.

Data availability

The data presented in this study are available in figshare47 at https://doi.org/10.6084/m9.figshare.16744258.

References

  1. US Department of Energy. Fuel Cell Technologies Office Multi-Year Research, Development, and Demonstration Plan Section 3.4 https://www.energy.gov/eere/fuelcells/articles/hydrogen-and-fuel-cell-technologies-office-multi-year-research-development (2016).

  2. Setzler, B. P., Zhuang, Z., Wittkopf, J. A. & Yan, Y. Activity targets for nanostructured platinum-group-metal-free catalysts in hydroxide exchange membrane fuel cells. Nat. Nanotechnol. 11, 1020–1025 (2016).

    Article  Google Scholar 

  3. Gu, S., Xu, B. & Yan, Y. Electrochemical energy engineering: a new frontier of chemical engineering innovation. Ann. Rev. Chem. Biomol. Eng. 5, 429–454 (2014).

    Article  Google Scholar 

  4. Campos-Roldán, C. A. & Alonso-Vante, N. The hydrogen oxidation reaction in alkaline medium: an overview. Electrochem. Energy Rev. 2, 312–331 (2019).

    Article  Google Scholar 

  5. Davydova, E. S., Mukerjee, S., Jaouen, F. & Dekel, D. R. Electrocatalysts for hydrogen oxidation reaction in alkaline electrolytes. ACS Catal. 8, 6665–6690 (2018).

    Article  Google Scholar 

  6. Ge, X. et al. Oxygen reduction in alkaline media: from mechanisms to recent advances of catalysts. ACS Catal. 5, 4643–4667 (2015).

    Article  Google Scholar 

  7. Zhang, J. et al. Recent insights on catalyst layers for anion exchange membrane fuel cells. Adv. Sci. https://doi.org/10.1002/advs.202100284 (2021).

  8. Huang, G. et al. Composite poly(norbornene) anion conducting membranes for achieving durability, water management and high power (3.4 W/cm2) in hydrogen/oxygen alkaline fuel cells. J. Electrochem. Soc. 166, F637–F644 (2019).

    Article  Google Scholar 

  9. Wang, L., Peng, X., Mustain, W. E. & Varcoe, J. R. Radiation-grafted anion-exchange membranes: the switch from low- to high-density polyethylene leads to remarkably enhanced fuel cell performance. Energy Environ. Sci. 12, 1575–1579 (2019).

    Article  Google Scholar 

  10. Wang, L., Bellini, M., Miller, H. A. & Varcoe, J. R. A high conductivity ultrathin anion-exchange membrane with 500+ h alkali stability for use in alkaline membrane fuel cells that can achieve 2 W cm−2 at 80 °C. J. Mater. Chem. A 6, 15404–15412 (2018).

    Article  Google Scholar 

  11. Chen, N. et al. Poly(alkyl-terphenyl piperidinium) ionomers and membranes with an outstanding alkaline-membrane fuel-cell performance of 2.58 W cm(-2). Angew. Chem. Int. Ed. Engl. 60, 7710–7718 (2021).

    Article  Google Scholar 

  12. Chen, N. et al. Poly(fluorenyl aryl piperidinium) membranes and ionomers for anion exchange membrane fuel cells. Nat. Commun. 12, 2367 (2021).

    Article  Google Scholar 

  13. Fan, J. et al. Poly(bis-arylimidazoliums) possessing high hydroxide ion exchange capacity and high alkaline stability. Nat. Commun. 10, 2306 (2019).

    Article  Google Scholar 

  14. Lee, W.-H., Kim, Y. S. & Bae, C. Robust hydroxide ion conducting poly(biphenyl alkylene)s for alkaline fuel cell membranes. ACS Macro Lett. 4, 814–818 (2015).

    Article  Google Scholar 

  15. Olsson, J. S., Pham, T. H. & Jannasch, P. Poly(arylene piperidinium) hydroxide ion exchange membranes: synthesis, alkaline stability, and conductivity. Adv. Funct. Mater. https://doi.org/10.1002/adfm.201702758 (2018).

  16. Wang, Y. et al. Synergistic Mn-Co catalyst outperforms Pt on high-rate oxygen reduction for alkaline polymer electrolyte fuel cells. Nat. Commun. 10, 1506 (2019).

    Article  Google Scholar 

  17. Adabi, H. et al. High-performing commercial Fe–N–C cathode electrocatalyst for anion-exchange membrane fuel cells. Nat. Energy 6, 834–843 (2021).

    Article  Google Scholar 

  18. Peng, X. et al. Nitrogen-doped carbon–CoOx nanohybrids: a precious metal free cathode that exceeds 1.0 W cm−2 peak power and 100 h life in anion-exchange membrane fuel cells. Angew. Chem. Int. Ed. 58, 1046–1051 (2019).

    Article  Google Scholar 

  19. Woo, J. et al. Promoting oxygen reduction reaction activity of Fe–N/C electrocatalysts by silica-coating-mediated synthesis for anion-exchange membrane fuel cells. Chem. Mater. 30, 6684–6701 (2018).

    Article  Google Scholar 

  20. Lu, Y. et al. Halloysite-derived nitrogen doped carbon electrocatalysts for anion exchange membrane fuel cells. J. Power Sources 372, 82–90 (2017).

    Article  Google Scholar 

  21. Xin, L., Zhang, Z., Wang, Z., Qi, J. & Li, W. Carbon supported Ag nanoparticles as high performance cathode catalyst for H2/O2 anion exchange membrane fuel cell. Front Chem. 1, 16 (2013).

    Article  Google Scholar 

  22. Peng, X. et al. Using operando techniques to understand and design high performance and stable alkaline membrane fuel cells. Nat. Commun. 11, 3561 (2020).

    Article  Google Scholar 

  23. Ul Hassan, N. et al. Achieving high‐performance and 2000 h stability in anion exchange membrane fuel cells by manipulating ionomer properties and electrode optimization. Adv. Energy Mater. https://doi.org/10.1002/aenm.202001986 (2020).

  24. Inaba, M. et al. Effects of carbon dioxide on the performance of anion-exchange membrane fuel cells. Electrochemistry 79, 322–325 (2011).

    Article  Google Scholar 

  25. Gerhardt, M. R., Pant, L. M. & Weber, A. Z. Along-the-channel impacts of water management and carbon-dioxide contamination in hydroxide-exchange-membrane fuel cells: a modeling study. J. Electrochem. Soc. 166, F3180–F3192 (2019).

    Article  Google Scholar 

  26. Zheng, Y. et al. Quantifying and elucidating the effect of CO2 on the thermodynamics, kinetics and charge transport of AEMFCs. Energy Environ. Sci. 12, 2806–2819 (2019).

    Article  Google Scholar 

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

    Article  Google Scholar 

  28. Caskey, S. R., Wong-Foy, A. G. & Matzger, A. J. Dramatic tuning of carbon dioxide uptake via metal substitution in a coordination polymer with cylindrical pores. J. Am. Chem. Soc. 130, 10870–10871 (2008).

    Article  Google Scholar 

  29. Shi, X. et al. Sorbents for the direct capture of CO2 from ambient air. Angew. Chem. Int. Ed. Engl. 59, 6984–7006 (2020).

    Article  Google Scholar 

  30. Yazaydın, A. Ö. et al. Screening of metal-organic frameworks for carbon dioxide capture from flue gas using a combined experimental and modeling approach. J. Am. Chem. Soc. 131, 18198–18199 (2009).

    Article  Google Scholar 

  31. Drese, J. H. et al. Synthesis–structure–property relationships for hyperbranched aminosilica CO2 adsorbents. Adv. Funct. Mater. 19, 3821–3832 (2009).

    Article  Google Scholar 

  32. Wurzbacher, J. A., Gebald, C., Piatkowski, N. & Steinfeld, A. Concurrent separation of CO2 and H2O from air by a temperature-vacuum swing adsorption/desorption cycle. Environ. Sci. Technol. 46, 9191–9198 (2012).

    Article  Google Scholar 

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

    Article  Google Scholar 

  34. Muroyama, A. P., Beard, A., Pribyl-Kranewitter, B. & Gubler, L. Separation of CO2 from dilute gas streams using a membrane electrochemical cell. ACS EST Eng. 1, 905–916 (2021).

    Article  Google Scholar 

  35. Muroyama, A. P., Pătru, A. & Gubler, L. Review—CO2 separation and transport via electrochemical methods. J. Electrochem. Soc. https://doi.org/10.1149/1945-7111/abbbb9 (2020).

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

    Article  Google Scholar 

  37. Rigdon, W. A. et al. Carbonate dynamics and opportunities with low temperature, anion exchange membrane-based electrochemical carbon dioxide separators. J. Electrochem. Energy Convers. Storage https://doi.org/10.1115/1.4033411 (2017).

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

    Article  Google Scholar 

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

    Article  Google Scholar 

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

    Article  Google Scholar 

  41. 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).

    Article  Google Scholar 

  42. 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).

    Article  Google Scholar 

  43. Matz, S. et al. Demonstration of electrochemically-driven CO2 separation using hydroxide exchange membranes. J. Electrochem. Soc. https://doi.org/10.1149/1945-7111/abd5fe (2021).

  44. Zheng, Y. et al. Editors’ choice—power-generating electrochemical CO2 scrubbing from air enabling practical AEMFC application. J. Electrochem. Soc. https://doi.org/10.1149/1945-7111/abe08a (2021).

  45. Baker, D. R., Caulk, D. A., Neyerlin, K. C. & Murphy, M. W. Measurement of oxygen transport resistance in PEM fuel cells by limiting current methods. J. Electrochem. Soc. 156, B991 (2009).

    Article  Google Scholar 

  46. Shi, L. et al. Editors’ choice—uncovering the role of alkaline pretreatment for hydroxide exchange membrane fuel cells. J. Electrochem. Soc. https://doi.org/10.1149/1945-7111/abc4bd (2020).

  47. Shi, L. et al. A shorted membrane electrochemical cell powered by hydrogen to remove CO2 from the air feed of hydroxide exchange membrane fuel cells. figshare https://doi.org/10.6084/m9.figshare.16744258 (2022).

  48. US Department of Energy Office of Energy Efficiency and Renewable Energy. Fuel Economy www.fueleconomy.gov (2021).

Download references

Acknowledgements

The information, data or work presented herein were funded in part by the Advanced Research Projects Agency-Energy (ARPA-E), US Department of Energy, under award number DE-AR0001034. S.G. is the principal investigator of the project. The views and opinions of authors expressed herein do not necessarily state or reflect those of the United States Government or any agency thereof.

Author information

Authors and Affiliations

Authors

Contributions

B.P.S. and Y.Y. conceived the idea of the shorted membrane and spiral-wound module. L.S. prepared the shorted membranes and designed the experiments. S.M. and B.P.S. designed the spiral-wound module. L.S. and Y.Z. characterized the shorted membranes, and fabricated and performed the single cell EDCS and spiral-wound module tests. B.P.S. developed the model of CO2 effect. B.P.S. and Y.Z. completed the technoeconomic analysis. S.G. provided guidance throughout the project, helped with data interpretation and improved the manuscript. L.S., Y.Z., B.P.S. and Y.Y. wrote the manuscript with the support of all co-authors.

Corresponding authors

Correspondence to Brian P. Setzler or Yushan Yan.

Ethics declarations

Competing interests

The PiperION membranes and ionomers were provided for free by Versogen, Inc. for which Y.Y., B.P.S. and Y.Z. are cofounders and S.G. is an adviser. L.S. and S.M. claim no competing interests.

Peer review

Peer review information

Nature Energy thanks Lorenz Gubler, Hamish Miller and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

Additional information

Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Supplementary information

Supplementary Information

Supplementary Notes 1–3, Tables 1–4 and Figs. 1–16.

Supplementary Video 1

Video showing demonstration of the spiral-wound EDCS module with different rates of hydrogen supply.

Rights and permissions

Reprints and Permissions

About this article

Verify currency and authenticity via CrossMark

Cite this article

Shi, L., Zhao, Y., Matz, S. et al. A shorted membrane electrochemical cell powered by hydrogen to remove CO2 from the air feed of hydroxide exchange membrane fuel cells. Nat Energy 7, 238–247 (2022). https://doi.org/10.1038/s41560-021-00969-5

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1038/s41560-021-00969-5

Further reading

Search

Quick links

Nature Briefing

Sign up for the Nature Briefing newsletter — what matters in science, free to your inbox daily.

Get the most important science stories of the day, free in your inbox. Sign up for Nature Briefing