Article

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

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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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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.

Author information

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.

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.

Corresponding author

Correspondence to James M. Tour.

Electronic supplementary material

  1. Supplementary Information

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