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Increased CO2 selectivity of asphalt-derived porous carbon through introduction of water into pore space

Nature Energy volume 2, pages 932–938 (2017)Cite this article

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Abstract

The development of inexpensive porous solid sorbents, such as porous carbons, that can selectively capture carbon dioxide (CO2) from natural gas wells is essential to reduce emission of CO2 to the atmosphere. However, at higher pressures, the selectivity for CO2 over that for methane (CH4) remains poor. Here we show that H2O can be imbibed within asphalt-derived porous carbon, with a surface area of 4,200 m2 g−1, to generate a hydrated powder material. While maintaining a high CO2 uptake capacity of 48 mmol g−1 (211 wt%), the molar selectivity for CO2 over CH4 increases to >200:1 and the H2O remains within the pores on repeated cycling. To mimic realistic natural gas wells, we used a 90% CH4 and 10% CO2 gas mixture and showed selective CO2 separation at 20 bar. Furthermore, in situ vibrational spectroscopy reveals the formation of an ordered matrix within the pores consisting of gas hydrates.

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Fig. 1: Preparation of \({\mathrm{uGilT}}_{{{\rm{H}}}_{{\rm{2}}}{\rm{O}}}\) and its gas sorption properties.
Fig. 2: Effects of temperature, equilibration time, water content and sorption–desorption cycling on CO2 sorption hysteresis.
Fig. 3: Selective CO2 uptake of \({\mathrm{uGilT}}_{{{\rm{H}}}_{{\rm{2}}}{\rm{O}}}\) from the 90% CH4 + 10% CO2 gas mixture.
Fig. 4: CO2 sorption isotherm and in situ vibrational spectroscopy.

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Acknowledgements

This work was graciously funded by Apache Corp. Prince Energy kindly provided the untreated Gilsonite. We thank J. Ho of Apache Corp. for helpful discussions on extensions to the industrial processes.

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Authors and Affiliations

  1. Department of Chemistry, Rice University, Houston, TX, USA

    Almaz S. Jalilov, Yilun Li, Carter Kittrell & James M. Tour

  2. Department of Chemistry and Center for Integrative Petroleum Research, King Fahd University of Petroleum and Minerals, Dhahran, Saudi Arabia

    Almaz S. Jalilov

  3. The NanoCarbon Center, Rice University, Houston, TX, USA

    Carter Kittrell & James M. Tour

  4. Department of Materials Science and NanoEngineering, Rice University, Houston, TX, USA

    James M. Tour

  5. Smalley-Curl Institute, Rice University, Houston, TX, USA

    James M. Tour

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Contributions

A.S.J. designed and performed the experiments and wrote the manuscript. Y.L. assisted with the experiments and analysis of gas sorption measurements. C.K. designed the high-pressure ATR-IR cell and helped with analyses of the IR data. J.M.T. oversaw all phases of the research and revised the manuscript. All authors discussed and commented on the manuscript.

Corresponding author

Correspondence to James M. Tour.

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Competing interests

Rice University has patent filings (PCT 62/209,489, WO 2017/035250 A1) on the carbon stationary phases and mechanisms described here for use in CO2 capture from natural gas. Apache Corp. has licensed the intellectual property. None of the authors owns rights to the technology described here and none holds stock in Apache Corp., aside from what might be held in broad mutual funds. All potential conflicts are disclosed to and managed by the Rice University Office of Sponsored Programs and Research Compliance.

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Supplementary Figures 1–16, Supplementary Tables 1–2, Supplementary References

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Jalilov, A.S., Li, Y., Kittrell, C. et al. Increased CO2 selectivity of asphalt-derived porous carbon through introduction of water into pore space. Nat Energy 2, 932–938 (2017). https://doi.org/10.1038/s41560-017-0030-y

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