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Liquid-based gating mechanism with tunable multiphase selectivity and antifouling behaviour

Abstract

Living organisms make extensive use of micro- and nanometre-sized pores as gatekeepers for controlling the movement of fluids, vapours and solids between complex environments. The ability of such pores to coordinate multiphase transport, in a highly selective and subtly triggered fashion and without clogging, has inspired interest in synthetic gated pores for applications ranging from fluid processing to 3D printing and lab-on-chip systems1,2,3,4,5,6,7,8,9,10. But although specific gating and transport behaviours have been realized by precisely tailoring pore surface chemistries and pore geometries6,11,12,13,14,15,16,17, a single system capable of controlling complex, selective multiphase transport has remained a distant prospect, and fouling is nearly inevitable11,12. Here we introduce a gating mechanism that uses a capillary-stabilized liquid as a reversible, reconfigurable gate that fills and seals pores in the closed state, and creates a non-fouling, liquid-lined pore in the open state. Theoretical modelling and experiments demonstrate that for each transport substance, the gating threshold—the pressure needed to open the pores—can be rationally tuned over a wide pressure range. This enables us to realize in one system differential response profiles for a variety of liquids and gases, even letting liquids flow through the pore while preventing gas from escaping. These capabilities allow us to dynamically modulate gas–liquid sorting in a microfluidic flow and to separate a three-phase air–water–oil mixture, with the liquid lining ensuring sustained antifouling behaviour. Because the liquid gating strategy enables efficient long-term operation and can be applied to a variety of pore structures and membrane materials, and to micro- as well as macroscale fluid systems, we expect it to prove useful in a wide range of applications.

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Figure 1: Hypothesis for gating a pore by liquid reconfiguration.
Figure 2: Design and rational tuning of gating systems with differentially controlled gas and liquid transport.
Figure 3: Sorting of multiphase mixtures by liquid-gated pores.
Figure 4: Antifouling transport and separation of complex substances.

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References

  1. Chen, P. C. & Xu, Z. K. Mineral-coated polymer membranes with superhydrophilicity and underwater superoleophobicity for effective oil/water separation. Sci. Rep. 3, 2776 (2013)

    Article  Google Scholar 

  2. Holt, J. K. et al. in Proc. 4th IEEE Conf. Nanotechnol. 110–112 (IEEE, 2004)

  3. Peng, X. S., Jin, J., Nakamura, Y., Ohno, T. & Ichinose, I. Ultrafast permeation of water through protein-based membranes. Nature Nanotechnol. 4, 353–357 (2009)

    Article  ADS  CAS  Google Scholar 

  4. Paven, M. et al. Super liquid-repellent gas membranes for carbon dioxide capture and heart-lung machines. Nature Commun. 4, 2512 (2013)

    Article  ADS  Google Scholar 

  5. Faulkner-Jones, A. et al. Development of a valve-based cell printer for the formation of human embryonic stem cell spheroid aggregates. Biofabrication 5, 015013 (2013)

    Article  ADS  CAS  Google Scholar 

  6. Oh, K. W. & Ahn, C. H. A review of microvalves. J. Micromech. Microeng. 16, R13–R39 (2006)

    Article  Google Scholar 

  7. Kargov, A. et al. in Proc. IEEE 9th Int. Conf. Rehabilitation Robotics 182–186 (IEEE, 2005)

  8. Edwards, D. A. et al. Large porous particles for pulmonary drug delivery. Science 276, 1868–1872 (1997)

    Article  CAS  Google Scholar 

  9. Kralj, J. G., Sahoo, H. R. & Jensen, K. F. Integrated continuous microfluidic liquid-liquid extraction. Lab Chip 7, 256–263 (2007)

    Article  CAS  Google Scholar 

  10. Karlsson, J. M. et al. Active liquid degassing in microfluidic systems. Lab Chip 13, 4366–4373 (2013)

    Article  CAS  Google Scholar 

  11. Ulbricht, M. Advanced functional polymer membranes. Polymer 47, 2217–2262 (2006)

    Article  CAS  Google Scholar 

  12. Lin, N. H., Kim, M. M., Lewis, G. T. & Cohen, Y. Polymer surface nano-structuring of reverse osmosis membranes for fouling resistance and improved flux performance. J. Mater. Chem. 20, 4642–4652 (2010)

    Article  CAS  Google Scholar 

  13. Powell, M. R., Cleary, L., Davenport, M., Shea, K. J. & Siwy, Z. S. Electric-field-induced wetting and dewetting in single hydrophobic nanopores. Nature Nanotechnol. 6, 798–802 (2011)

    Article  ADS  CAS  Google Scholar 

  14. Yameen, B. et al. Ionic transport through single solid-state nanopores controlled with thermally nanoactuated macromolecular gates. Small 5, 1287–1291 (2009)

    Article  CAS  Google Scholar 

  15. Wen, Y. Q. et al. DNA-based intelligent logic controlled release systems. Chem. Commun. 48, 8410–8412 (2012)

    Article  CAS  Google Scholar 

  16. Adrus, N. & Ulbricht, M. Novel hydrogel pore-filled composite membranes with tunable and temperature-responsive size-selectivity. J. Mater. Chem. 22, 3088–3098 (2012)

    Article  CAS  Google Scholar 

  17. 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)

    Article  ADS  CAS  Google Scholar 

  18. Stroock, A. D., Pagay, V. V., Zwieniecki, M. A. & Holbrook, N. M. The physicochemical hydrodynamics of vascular plants. Annu. Rev. Fluid Mech. 46, 615–642 (2014)

    Article  ADS  MathSciNet  MATH  Google Scholar 

  19. Peleg, O. & Lim, R. Y. H. Converging on the function of intrinsically disordered nucleoporins in the nuclear pore complex. Biol. Chem. 391, 719–730 (2010)

    Article  CAS  Google Scholar 

  20. Namati, E., Thiesse, J., de Ryk, J. & McLennan, G. Alveolar dynamics during respiration: are the pores of Kohn a pathway to recruitment? Am. J. Respir. Cell Mol. Biol. 38, 572–578 (2008)

    Article  CAS  Google Scholar 

  21. Winther-Jensen, B., Winther-Jensen, O., Forsyth, M. & Macfarlane, D. R. High rates of oxygen reduction over a vapor phase-polymerized PEDOT electrode. Science 321, 671–674 (2008)

    Article  ADS  CAS  Google Scholar 

  22. Mohns, J. & Kunnecke, W. Flow-analysis with membrane separation and time-based sampling for ethanol determination in beer and wine. Anal. Chim. Acta 305, 241–247 (1995)

    Article  CAS  Google Scholar 

  23. Liu, C. C., Thompson, J. A. & Bau, H. H. A membrane-based, high-efficiency, microfluidic debubbler. Lab Chip 11, 1688–1693 (2011)

    Article  CAS  Google Scholar 

  24. Yusko, E. C. et al. Controlling protein translocation through nanopores with bio-inspired fluid walls. Nature Nanotechnol. 6, 253–260 (2011)

    Article  ADS  CAS  Google Scholar 

  25. Wong, T. S. et al. Bioinspired self-repairing slippery surfaces with pressure-stable omniphobicity. Nature 477, 443–447 (2011)

    Article  ADS  CAS  Google Scholar 

  26. Mietton-Peuchot, M., Condat, C. & Courtois, T. Use of gas-liquid porometry measurements for selection of microfiltration membranes. J. Membr. Sci. 133, 73–82 (1997)

    Article  CAS  Google Scholar 

  27. Zhang, C. Y., Oostrom, M., Wietsma, T. W., Grate, J. W. & Warner, M. G. Influence of viscous and capillary forces on immiscible fluid displacement: pore-scale experimental study in a water-wet micromodel demonstrating viscous and capillary fingering. Energy Fuels 25, 3493–3505 (2011)

    Article  CAS  Google Scholar 

  28. Germic, L. et al. Characterization of polyacrylonitrile ultrafiltration membranes. J. Membr. Sci. 132, 131–145 (1997)

    Article  CAS  Google Scholar 

  29. Biot, M. A. General theory of three-dimensional consolidation. J. Appl. Phys. 12, 155–164 (1941)

    Article  ADS  MATH  Google Scholar 

  30. Purcell, W. R. Capillary pressures - their measurement using mercury and the calculation of permeability therefrom. J. Petrol. Technol. 1, 39–48 (1949)

    Article  CAS  Google Scholar 

Download references

Acknowledgements

This work was supported in part by the Advanced Research Projects Agency-Energy (ARPA-E), US Department of Energy, under award number DE-AR0000326. We thank M. Aizenberg, R. T. Blough and X. Y. Chen for discussions; A. B. Tesler for assistance with the scanning electron microscopy; and T. S. Wong, B. D. Hatton and R. A. Belisle for assistance with antifouling experiments.

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Authors and Affiliations

Authors

Contributions

X.H. and J.A. designed the liquid-infused porous materials and the experiments. X.H. and M.K. carried out the experiments. All authors analysed data. Y.H. built the mathematical model. All authors interpreted data and wrote the paper.

Corresponding author

Correspondence to Joanna Aizenberg.

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The authors declare no competing financial interests.

Supplementary information

Supplementary Information

This file contains Supplementary Methods, Supplementary Tables 1-4, Supplementary Figures 1-16, Supplementary Text & Data and Supplementary Results & Discussion. (PDF 3145 kb)

Rapid pressure-tunable sorting of multiphase flows in a microfluidic system and longevity testing

A liquid-gated membrane incorporated into a port along a microfluidic channel enables a series of distinct pressure-dependent scenarios for a mixed air/water flow. Below both Pcritical(air) and Pcritical(water), nothing crosses the port. Above Pcritical(air)) and below Pcritical(water), only air flows through the port and degassed water continues through the channel beyond the port. Above both Pcritical(air) and Pcritical(water), both phases cross the port and only water continues through the channel. Above both critical pressures, the water:air ratio that crosses the port increases with increasing pressure. This behavior remains robust for at least six days of continuous operation (flow rates 5-1000 µL/min). (MP4 12677 kb)

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Hou, X., Hu, Y., Grinthal, A. et al. Liquid-based gating mechanism with tunable multiphase selectivity and antifouling behaviour. Nature 519, 70–73 (2015). https://doi.org/10.1038/nature14253

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