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.

  • Letter
  • Published:

Joule-heated graphene-wrapped sponge enables fast clean-up of viscous crude-oil spill

Nature Nanotechnology volume 12, pages 434–440 (2017)Cite this article

Subjects

Abstract

The clean-up of viscous crude-oil spills is a global challenge. Hydrophobic and oleophilic oil sorbents have been demonstrated as promising candidates for oil-spill remediation. However, the sorption speeds of these oil sorbents for viscous crude oil are rather limited. Herein we report a Joule-heated graphene-wrapped sponge (GWS) to clean-up viscous crude oil at a high sorption speed. The Joule heat of the GWS reduced in situ the viscosity of the crude oil, which prominently increased the oil-diffusion coefficient in the pores of the GWS and thus speeded up the oil-sorption rate. The oil-sorption time was reduced by 94.6% compared with that of non-heated GWS. Besides, the oil-recovery speed was increased because of the viscosity decrease of crude oil. This in situ Joule self-heated sorbent design will promote the practical application of hydrophobic and oleophilic oil sorbents in the clean-up of viscous crude-oil spills.

This is a preview of subscription content, access via your institution

Access options

Buy this article

  • Purchase on Springer Link
  • Instant access to full article PDF
Buy now

Prices may be subject to local taxes which are calculated during checkout

Figure 1: Schematic illustration of Joule-heated GWS used to clean-up a viscous crude-oil spill.
Figure 2: Fabrication of the GWS and Joule-heating effect of the GWS.
Figure 3: Effect of Joule heating on the oil-sorption kinetics.
Figure 4: Effects of heat distribution on the utilization efficiency of heat energy.
Figure 5: Influence of Joule heat on the oil-recovery speed.

Similar content being viewed by others

References

  1. Jernelov, A. How to defend against future oil spills. Nature 466, 182–183 (2010).

    Article  Google Scholar 

  2. Peterson, C. H. et al. Long-term ecosystem response to the Exxon Valdez oil spill. Science 302, 2082–2086 (2003).

    Article  CAS  Google Scholar 

  3. Kujawinski, E. B. et al. Fate of dispersants associated with the Deepwater Horizon oil spill. Environ. Sci. Technol. 45, 1298–1306 (2011).

    Article  CAS  Google Scholar 

  4. Vidyasagar, A., Handore, K. & Sureshan, K. M. Soft optical devices from self-healing gels formed by oil and sugar-based organogelators. Angew. Chem. Int. Ed. 50, 8021–8024 (2011).

    Article  CAS  Google Scholar 

  5. Buist, I., McCourt, J., Potter, S., Ross, S. & Trudel, K. In situ burning. Pure Appl. Chem. 71, 43–65 (1999).

    Article  CAS  Google Scholar 

  6. Broje, V. & Keller, A. A. Improved mechanical oil spill recovery using an optimized geometry for the skimmer surface. Environ. Sci. Technol. 40, 7914–7918 (2006).

    Article  CAS  Google Scholar 

  7. Sun, H., Xu, Z. & Gao, C. Multifunctional, ultra-flyweight, synergistically assembled carbon aerogels. Adv. Mater. 25, 2554–2560 (2013).

    Article  CAS  Google Scholar 

  8. Si, Y., Yu, J., Tang, X., Ge, J. & Ding, B. Ultralight nanofibre-assembled cellular aerogels with superelasticity and multifunctionality. Nat. Commun. 5, 5802 (2014).

    Article  Google Scholar 

  9. Barg, S. et al. Mesoscale assembly of chemically modified graphene into complex cellular networks. Nat. Commun. 5, 4328 (2014).

    Article  CAS  Google Scholar 

  10. Wu, C., Huang, X., Wu, X., Qian, R. & Jiang, P. Mechanically flexible and multifunctional polymer-based graphene foams for elastic conductors and oil–water separators. Adv. Mater. 25, 5658–5662 (2013).

    Article  CAS  Google Scholar 

  11. Niu, Z., Chen, J., Hng, H. H., Ma, J. & Chen, X. A leavening strategy to prepare reduced graphene oxide foams. Adv. Mater. 24, 4144–4150 (2012).

    Article  CAS  Google Scholar 

  12. Wu, Z.-Y. et al. Carbon nanofiber aerogels for emergent cleanup of oil spillage and chemical leakage under harsh conditions. Sci. Rep. 4, 4079 (2014).

    Article  Google Scholar 

  13. Liang, H.-W. et al. Macroscopic-scale template synthesis of robust carbonaceous nanofiber hydrogels and aerogels and their applications. Angew. Chem. Int. Ed. 51, 5101–5105 (2012).

    Article  CAS  Google Scholar 

  14. Bi, H. et al. Spongy graphene as a highly efficient and recyclable sorbent for oils and organic solvents. Adv. Funct. Mater. 22, 4421–4425 (2012).

    Article  CAS  Google Scholar 

  15. Lei, W. W., Portehault, D., Liu, D., Qin, S. & Chen, Y. Porous boron nitride nanosheets for effective water cleaning. Nat. Commun. 4, 1777 (2013).

    Article  Google Scholar 

  16. Yuan, J. et al. Superwetting nanowire membranes for selective absorption. Nat. Nanotech. 3, 332–336 (2008).

    Article  CAS  Google Scholar 

  17. Ruan, C., Ai, K., Li, X. & Lu, L. A superhydrophobic sponge with excellent absorbency and flame retardancy. Angew. Chem. Int. Ed. 53, 5556–5560 (2014).

    Article  CAS  Google Scholar 

  18. Nguyen, D. D., Tai, N.-H., Lee, S.-B. & Kuo, W.-S. Superhydrophobic and superoleophilic properties of graphene-based sponges fabricated using a facile dip coating method. Energy Environ. Sci. 5, 7908–7912 (2012).

    Article  CAS  Google Scholar 

  19. Hayase, G., Kanamori, K., Fukuchi, M., Kaji, H. & Nakanishi, K. Facile synthesis of marshmallow-like macroporous gels usable under harsh conditions for the separation of oil and water. Angew. Chem. Int. Ed. 52, 1986–1989 (2013).

    Article  CAS  Google Scholar 

  20. Ge, J. et al. Pumping through porous hydrophobic/oleophilic materials: an alternative technology for oil spill remediation. Angew. Chem. Int. Ed. 53, 3612–3616 (2014).

    Article  CAS  Google Scholar 

  21. Fingas, M. F. The evaporation of oil spills: development and implementation of new prediction methodology. In Int. Oil Spill Conf. Proc. 281–287 (1999).

    Article  Google Scholar 

  22. Pei, S., Zhao, J., Du, J., Ren, W. & Cheng, H.-M. Direct reduction of graphene oxide films into highly conductive and flexible graphene films by hydrohalic acids. Carbon 48, 4466–4474 (2010).

    Article  CAS  Google Scholar 

  23. Stankovich, S. et al. Synthesis of graphene-based nanosheets via chemical reduction of exfoliated graphite oxide. Carbon 45, 1558–1565 (2007).

    Article  CAS  Google Scholar 

  24. Trung, T. Q. et al. High thermal responsiveness of a reduced graphene oxide field-effect transistor. Adv. Mater. 24, 5254–5260 (2012).

    Article  CAS  Google Scholar 

  25. Wang, Z.-L. et al. Facile, mild and fast thermal-decomposition reduction of graphene oxide in air and its application in high-performance lithium batteries. Chem. Commun. 48, 976–978 (2012).

    Article  CAS  Google Scholar 

  26. Liao, A. D. et al. Thermally limited current carrying ability of graphene nanoribbons. Phys. Rev. Lett. 106, 256801 (2011).

    Article  Google Scholar 

  27. Aggarwal, R. K. Evaluation of relative wettability of carbon-fibers. Carbon 15, 291–293 (1977).

    Article  CAS  Google Scholar 

  28. Nishi, Y., Dai, G. Z., Iwashita, N., Sawada, Y. & Inagaki, M. Evaluation of sorption behavior of heavy oil into exfoliated graphite by wicking test. Mater. Sci. Res. Int. 8, 243–248 (2002).

    CAS  Google Scholar 

  29. Nishi, Y., Iwashita, N., Sawada, Y. & Inagaki, M. Sorption kinetics of heavy oil into porous carbons. Water Res. 36, 5029–5036 (2002).

    Article  CAS  Google Scholar 

  30. Beltran, V., Escardino, A., Feliu, C. & Rodrigo, M. D. Liquid suction by porous ceramic materials. Br. Ceram. Trans. 87, 64–69 (1988).

    CAS  Google Scholar 

  31. Ge, J. et al. Facile dip coating processed graphene/MnO2 nanostructured sponges as high performance supercapacitor electrodes. Nano Energy 2, 505–513 (2013).

    Article  CAS  Google Scholar 

Download references

Acknowledgements

This work is supported by the Foundation for Innovative Research Groups of the National Natural Science Foundation of China (Grant 21521001), the National Natural Science Foundation of China (Grants 21431006, 21761132008 and 11525211), Key Research Program of Frontier Sciences, CAS (Grant QYZDJ-SSW-SLH036), the Chinese Academy of Sciences (Grants KFJ-EW-116, KJZD-EW-M01-1), the Strategic Priority Research Program of the Chinese Academy of Sciences (XDB22040402), the Ministry of Science and Technology of China (Grant 2014CB931800), the Users with Excellence and Scientific Research Grant of Hefei Science Center of CAS (2015HSC-UE007) and the Fundamental Research Funds for the Central Universities (WK6030000018). We thank H.-L. Jiang for help in obtaining the crude oil provided by the China University of Petroleum (Huadong).

Author information

Author notes

  1. Jin Ge, Lu-An Shi and Yong-Chao Wang: These authors contribute equally to this work

Authors and Affiliations

  1. Division of Nanomaterials and Chemistry, Department of Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Suzhou Nano Science and Technology, CAS Center for Excellence in Nanoscience, Hefei Science Center of CAS, University of Science and Technology of China, Hefei, 230026, China

    Jin Ge, Lu-An Shi, Hao-Yu Zhao, Hong-Bin Yao, Ye Zhang, Hong-Wu Zhu & Shu-Hong Yu

  2. Department of Modern Mechanics, CAS Key Laboratory of Mechanical Behavior and Design of Materials, CAS Center for Excellence in Nanoscience, University of Science and Technology of China, Hefei, 230027, Anhui, China

    Yong-Chao Wang, Yin-Bo Zhu & Heng-An Wu

Authors
  1. Jin Ge
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Lu-An Shi
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Yong-Chao Wang
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Hao-Yu Zhao
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Hong-Bin Yao
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Yin-Bo Zhu
    View author publications

    You can also search for this author in PubMed Google Scholar

  7. Ye Zhang
    View author publications

    You can also search for this author in PubMed Google Scholar

  8. Hong-Wu Zhu
    View author publications

    You can also search for this author in PubMed Google Scholar

  9. Heng-An Wu
    View author publications

    You can also search for this author in PubMed Google Scholar

  10. Shu-Hong Yu
    View author publications

    You can also search for this author in PubMed Google Scholar

Contributions

J.G. and S.-H.Y. conceived the idea and designed the experiments. J.G. planned the experiments, performed the experiments, collected and analysed the data, and wrote the paper. S.-H.Y. supervised the project, analysed the results and wrote the paper. L.-A.S. designed and performed the experiments, and collected and analysed the data. H.-A.W. supervised the simulations of heat transfer. Y.-C.W. and Y.-B.Z. performed the simulations and wrote the paper, and contributed to the discussion of energy utilization and optimization design. H.-Y.Z., Y.Z. and H.-W.Z. designed and performed the experiments. H.-B.Y. analysed the results and wrote the paper. All authors discussed the results and commented on the manuscript.

Corresponding author

Correspondence to Shu-Hong Yu.

Ethics declarations

Competing interests

The authors declare no competing financial interests.

Supplementary information

Supplementary information

Supplementary information (PDF 2082 kb)

Supplementary Movie 1

Supplementary Movie 1 (MP4 4092 kb)

Supplementary Movie 2

Supplementary Movie 2 (MP4 10160 kb)

Supplementary Movie 3

Supplementary Movie 3 (MP4 5523 kb)

Supplementary Movie 4

Supplementary Movie 4 (GIF 2067 kb)

Supplementary Movie 5

Supplementary Movie 5 (MP4 3207 kb)

Supplementary Movie 6

Supplementary Movie 6 (MP4 5457 kb)

Supplementary Movie 7

Supplementary Movie 7 (MP4 7012 kb)

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Ge, J., Shi, LA., Wang, YC. et al. Joule-heated graphene-wrapped sponge enables fast clean-up of viscous crude-oil spill. Nature Nanotech 12, 434–440 (2017). https://doi.org/10.1038/nnano.2017.33

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1038/nnano.2017.33

This article is cited by

Search

Advanced 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