Abstract

Superfast water transport discovered in graphitic nanoconduits, including carbon nanotubes and graphene nanochannels, implicates crucial applications in separation processes and energy conversion. Yet lack of complete understanding at the single-conduit level limits development of new carbon nanofluidic structures and devices with desired transport properties for practical applications. Here, we show that the hydraulic resistance and slippage of single graphene nanochannels can be accurately determined using capillary flow and a novel hybrid nanochannel design without estimating the capillary pressure. Our results reveal that the slip length of graphene in the graphene nanochannels is around 16 nm, albeit with a large variation from 0 to 200 nm regardless of the channel height. We corroborate this finding with molecular dynamics simulation results, which indicate that this wide distribution of the slip length is due to the surface charge of graphene as well as the interaction between graphene and its silica substrate.

Access optionsAccess options

Rent or Buy article

Get time limited or full article access on ReadCube.

from$8.99

All prices are NET prices.

Additional information

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

References

  1. 1.

    Majumder, M., Chopra, N., Andrews, R. & Hinds, B. J. Nanoscale hydrodynamics: enhanced flow in carbon nanotubes. Nature 438, 44 (2005).

  2. 2.

    Holt, J. K. et al. Fast mass transport through sub-2-nanometer carbon nanotubes. Science 312, 1034–1037 (2006).

  3. 3.

    Nair, R. R., Wu, H. A., Jayaram, P. N., Grigorieva, I. V. & Geim, A. K. Unimpeded permeation of water through helium-leak–tight graphene-based membranes. Science 335, 442–444 (2012).

  4. 4.

    Huang, H. et al. Ultrafast viscous water flow through nanostrand-channelled graphene oxide membranes. Nat. Commun. 4, 2979 (2013).

  5. 5.

    Radha, B. et al. Molecular transport through capillaries made with atomic-scale precision. Nature 538, 222–225 (2016).

  6. 6.

    Corry, B. Designing carbon nanotube membranes for efficient water desalination. J. Phys. Chem. B 112, 1427–1434 (2008).

  7. 7.

    Das, R., Ali, M. E., Hamid, S. B. A., Ramakrishna, S. & Chowdhury, Z. Z. Carbon nanotube membranes for water purification: A bright future in water desalination. Desalination 336, 97–109 (2014).

  8. 8.

    Cohen-Tanugi, D. & Grossman, J. C. Water desalination across nanoporous graphene. Nano Lett. 12, 3602–3608 (2012).

  9. 9.

    Surwade, S. P. et al. Water desalination using nanoporous single-layer graphene. Nat. Nanotech. 10, 459–464 (2015).

  10. 10.

    Kim, H. W. et al. Selective gas transport through few-layered graphene and graphene oxide membranes. Science 342, 91–95 (2013).

  11. 11.

    Li, H. et al. Ultrathin, molecular-sieving graphene oxide membranes for selective hydrogen separation. Science 342, 95–98 (2013).

  12. 12.

    Joshi, R. K. et al. Precise and ultrafast molecular sieving through graphene oxide membranes. Science 343, 752–754 (2014).

  13. 13.

    Candelaria, S. L. et al. Nanostructured carbon for energy storage and conversion. Nano Energy 1, 195–220 (2012).

  14. 14.

    Park, H. G. & Jung, Y. Carbon nanofluidics of rapid water transport for energy applications. Chem. Soc. Rev. 43, 565–576 (2014).

  15. 15.

    Xie, Q., Xin, F., Park, H. G. & Duan, C. Ion transport in graphene nanofluidic channels. Nanoscale 8, 19527–19535 (2016).

  16. 16.

    Yongqiang, R. & Derek, S. Slip-enhanced electrokinetic energy conversion in nanofluidic channels. Nanotechnology 19, 195707 (2008).

  17. 17.

    Qin, X., Yuan, Q., Zhao, Y., Xie, S. & Liu, Z. Measurement of the rate of water translocation through carbon nanotubes. Nano Lett. 11, 2173–2177 (2011).

  18. 18.

    Secchi, E. et al. Massive radius-dependent flow slippage in carbon nanotubes. Nature 537, 210–213 (2016).

  19. 19.

    Wei, N., Peng, X. & Xu, Z. Understanding water permeation in graphene oxide membranes. ACS Appl. Mater. Interfaces 6, 5877–5883 (2014).

  20. 20.

    Boukhvalov, D. W., Katsnelson, M. I. & Son, Y.-W. Origin of anomalous water permeation through graphene oxide membrane. Nano Lett. 13, 3930–3935 (2013).

  21. 21.

    Muscatello, J., Jaeger, F., Matar, O. K. & Müller, E. A. Optimizing water transport through graphene-based membranes: insights from nonequilibrium molecular dynamics. ACS Appl. Mater. Interfaces 8, 12330–12336 (2016).

  22. 22.

    Alibakhshi, M. A., Xie, Q., Li, Y. & Duan, C. Accurate measurement of liquid transport through nanoscale conduits. Sci. Rep. 6, 24936 (2016).

  23. 23.

    Tas, N. R., Haneveld, J., Jansen, H. V., Elwenspoek, M. & van den Berg, A. Capillary filling speed of water in nanochannels. Appl. Phys. Lett. 85, 3274–3276 (2004).

  24. 24.

    Haneveld, J., Tas, N. R., Brunets, N., Jansen, H. V. & Elwenspoek, M. Capillary filling of sub-10nm nanochannels. J. Appl. Phys. 104, 014309 (2008).

  25. 25.

    Mortensen, N. A. & Kristensen, A. Electroviscous effects in capillary filling of nanochannels. Appl. Phys. Lett. 92, 063110 (2008).

  26. 26.

    Phan, V.-N., Yang, C. & Nguyen, N.-T. Analysis of capillary filling in nanochannels with electroviscous effects. Microfluid. Nanofluid. 7, 519–530 (2009).

  27. 27.

    Wang, M., Chang, C.-C. & Yang, R.-J. Electroviscous effects in nanofluidic channels. J. Chem. Phys. 132, 024701 (2010).

  28. 28.

    Hong, J.-Y. et al. A rational strategy for graphene transfer on substrates with rough features. Adv. Mater. 28, 2382–2392 (2016).

  29. 29.

    Huang, W., Liu, Q. & Li, Y. Capillary filling flows inside patterned‐surface microchannels. Chem. Eng. Technol. 29, 716–723 (2006).

  30. 30.

    Sendner, C., Horinek, D., Bocquet, L. & Netz, R. R. Interfacial water at hydrophobic and hydrophilic surfaces: slip, viscosity, and diffusion. Langmuir 25, 10768–10781 (2009).

  31. 31.

    Goertz, M. P., Houston, J. E. & Zhu, X. Y. Hydrophilicity and the viscosity of interfacial water. Langmuir 23, 5491–5497 (2007).

  32. 32.

    Li, T.-D., Gao, J., Szoszkiewicz, R., Landman, U. & Riedo, E. Structured and viscous water in subnanometer gaps. Phys. Rev. B 75, 115415 (2007).

  33. 33.

    Secchi, E., Niguès, A., Jubin, L., Siria, A. & Bocquet, L. Scaling behavior for ionic transport and its fluctuations in individual carbon nanotubes. Phys. Rev. Lett. 116, 154501 (2016).

  34. 34.

    Ambrosi, A., Chua, C. K., Bonanni, A. & Pumera, M. Electrochemistry of graphene and related materials. Chem. Rev. 114, 7150–7188 (2014).

  35. 35.

    Ping, J. & Johnson, A. T. C. Quantifying the intrinsic surface charge density and charge-transfer resistance of the graphene-solution interface through bias-free low-level charge measurement. Appl. Phys. Lett. 109, 013103 (2016).

  36. 36.

    Chen, F., Qing, Q., Xia, J., Li, J. & Tao, N. Electrochemical gate-controlled charge transport in graphene in ionic liquid and aqueous solution. J. Am. Chem. Soc. 131, 9908–9909 (2009).

  37. 37.

    Zhong, J.-H. et al. Quantitative correlation between defect density and heterogeneous electron transfer rate of single layer graphene. J. Am. Chem. Soc. 136, 16609–16617 (2014).

  38. 38.

    Rafiee, J. et al. Wetting transparency of graphene. Nat. Mater. 11, 217–222 (2012).

  39. 39.

    Shih, C.-J. et al. Breakdown in the wetting transparency of graphene. Phys. Rev. Lett. 109, 176101 (2012).

  40. 40.

    Shih, C.-J., Strano, M. S. & Blankschtein, D. Wetting translucency of graphene. Nat. Mater. 12, 866–869 (2013).

  41. 41.

    Maali, A., Cohen-Bouhacina, T. & Kellay, H. Measurement of the slip length of water flow on graphite surface. Appl. Phys. Lett. 92, 053101 (2008).

  42. 42.

    Thomas, J. A. & McGaughey, A. J. H. Reassessing fast water transport through carbon nanotubes. Nano Lett. 8, 2788–2793 (2008).

  43. 43.

    Kumar Kannam, S., Todd, B. D., Hansen, J. S. & Daivis, P. J. Slip length of water on graphene: limitations of non-equilibrium molecular dynamics simulations. J. Chem. Phys. 136, 024705 (2012).

  44. 44.

    Falk, K., Sedlmeier, F., Joly, L., Netz, R. R. & Bocquet, L. Molecular origin of fast water transport in carbon nanotube membranes: superlubricity versus curvature dependent friction. Nano Lett. 10, 4067–4073 (2010).

  45. 45.

    Plimpton, S. Fast parallel algorithms for short-range molecular dynamics. J. Comput. Phys. 117, 1–19 (1995).

  46. 46.

    Shih, C.-J., Lin, S., Sharma, R., Strano, M. S. & Blankschtein, D. Understanding the pH-dependent behavior of graphene oxide aqueous solutions: a comparative experimental and molecular dynamics simulation study. Langmuir 28, 235–241 (2012).

  47. 47.

    Wei, N., Lv, C. & Xu, Z. Wetting of graphene oxide: a molecular dynamics study. Langmuir 30, 3572–3578 (2014).

  48. 48.

    Hockney, R. W. & Eastwood, J. W. Computer Simulation Using Particles (Taylor & Francis, New York, 1988).

Download references

Acknowledgements

This work is supported by the Faculty Startup Fund (Boston University, USA) and the NSF Faculty Early Career Development (CAREER) programme award (CBET-1653767). The authors would like to thank the Photonics Center at Boston University for the use of their fabrication and characterization facilities. S.J. and Z.X. acknowledge the support from the National Natural Science Foundation of China through grant no. 11472150. M.H. and J.K. are thankful for financial support by the AFOSR FATE MURI, grant no. FA9550-15-1-0514. H.G.P. appreciates the support from ETH grant (ETH-30 13-1) and Swiss National Science Foundation (200021-146856).

Author information

Affiliations

  1. Department of Mechanical Engineering, Boston University, Boston, MA, USA

    • Quan Xie
    • , Mohammad Amin Alibakhshi
    •  & Chuanhua Duan
  2. Department of Engineering Mechanics and Center for Nano and Micro Mechanics, Tsinghua University, Beijing, China

    • Shuping Jiao
    •  & Zhiping Xu
  3. Department of Electrical Engineering and Computer Science, Massachusetts Institute of Technology, Cambridge, MA, USA

    • Marek Hempel
    •  & Jing Kong
  4. Department of Mechanical and Process Engineering, Eidgenössische Technische Hochschule (ETH) Zürich, Zürich, Switzerland

    • Hyung Gyu Park

Authors

  1. Search for Quan Xie in:

  2. Search for Mohammad Amin Alibakhshi in:

  3. Search for Shuping Jiao in:

  4. Search for Zhiping Xu in:

  5. Search for Marek Hempel in:

  6. Search for Jing Kong in:

  7. Search for Hyung Gyu Park in:

  8. Search for Chuanhua Duan in:

Contributions

C.D. conceived the idea and directed the project; C.D., Q.X. and M.A. designed the experiments; Q.X. fabricated the nanofluidic devices and performed the experiments; Q.X. and M.A. analysed the experimental data; S.J. and Z.X. performed the MD simulations; M.H., J.K. and H.G.P. provided graphene samples; C.D., Q.X. and Z.X. wrote the manuscript. All authors participated in completing the manuscript.

Competing interests

The authors declare no competing financial interests.

Corresponding author

Correspondence to Chuanhua Duan.

Supplementary information

  1. Supplementary Information

    Supplementary Figs. 1–10, Supplementary Tables 1–3, Supplementary References.

Videos

  1. Supplementary Video 1

    Supplementary Video 1.

  2. Supplementary Video 2

    Supplementary Video 2.

  3. Supplementary Video 3

    Supplementary Video 3.

About this article

Publication history

Received

Accepted

Published

DOI

https://doi.org/10.1038/s41565-017-0031-9