Science - USA (2022-06-03)

(Antfer) #1

spectrum peak relative to the permeate still
broad but shifted to lower mass values. The
permeate obtained in the first stage was
utilized as feed in the second stage using the
more cross-linked D325-1h membrane with a
tighter layer. The GC chromatogram shows
that more than 90% of the hydrocarbons
with carbon numbers below C 10 were con-
centrated in the permeate side (Fig. 4D).
The results reported here show that by
rationally selecting the polymer structure and
combining the classical NIPS method with
thermal cross-linking, it is possible to obtain
promising membranes for a highly challeng-
ing chemical separation: the fractionation of
crude oil. The versatility of the polytriazole in
terms of processability and cross-linking allows
polymeric membranes to be obtained with a
tailored selective layer by using a method that
is easy to scale up. The tunable selectivity and
permeances of the ultrathin polytriazole layer
make these membranes suitable for a cascade
system with each step providing a specific range
of hydrocarbon separations. High thermal
stability permits testing feed mixtures in dif-
ferent conditions that other polymeric mem-
branes may not be able towithstand, suggesting
that the polytriazole membranes can be in-
tegrated into hybrid membrane configurations
for energy-efficient crude oil fractionation.


REFERENCES AND NOTES



  1. P. Marchetti, M. F. Jimenez Solomon, G. Szekely,
    A. G. Livingston,Chem. Rev. 114 , 10735–10806 (2014).

  2. D. S. Sholl, R. P. Lively,Nature 532 , 435–437 (2016).
    3. R. P. Lively, D. S. Sholl,Nat. Mater. 16 , 276–279 (2017).
    4. P. Vandezande, L. E. M. Gevers, I. F. J. Vankelecom,
    Chem. Soc. Rev. 37 , 365–405 (2008).
    5. H. B. Park, J. Kamcev, L. M. Robeson, M. Elimelech,
    B. D. Freeman,Science 356 , eaab0530 (2017).
    6. S. P. Nuneset al., J. Membr. Sci. 598 , 117761 (2020).
    7. W. J. Koros, C. Zhang,Nat. Mater. 16 , 289–297 (2017).
    8. B. Van der Bruggen, inMembrane Operations: Innovative
    Separations and Transformations(Wiley, 2009), pp. 4561.
    9. K. Vanherck, G. Koeckelberghs, I. F. J. Vankelecom,
    Prog. Polym. Sci. 38 , 874–896 (2013).
    10. J. da Silva Burgal, L. Peeva, A. Livingston,J. Membr. Sci. 525 ,
    48 – 56 (2017).
    11. M. Cook, P. R. J. Gaffney, L. G. Peeva, A. G. Livingston,
    J. Membr. Sci. 558 ,52–63 (2018).
    12. K. A. Thompsonet al., Science 369 , 310–315 (2020).
    13. J. F. Brennecke, B. Freeman,Science 369 , 254–255 (2020).
    14. S. Chisca, G. Falca, V. E. Musteata, C. Boi, S. P. Nunes,
    J. Membr. Sci. 528 , 264–272 (2017).
    15. E. Jinet al., Science 357 , 673–676 (2017).
    16. S. Chiscaet al., J. Membr. Sci. 597 , 117634 (2020).
    17. M. Chowdhury, R. D. Priestley,Proc. Natl. Acad. Sci. U.S.A. 114 ,
    4854 – 4856 (2017).
    18. S.-H. Parket al., Green Chem. 23 , 1175–1184 (2021).
    19. J. M. Bernal-García, A. Guzmán-López, A. Cabrales-Torres,
    A. Estrada-Baltazar, G. A. Iglesias-Silva,J. Chem. Eng. Data 53 ,
    1024 – 1027 (2008).
    20. J. H. Kimet al., Green Chem. 20 , 1887–1898 (2018).
    21. S. Darvishmanesh, J. Degrève, B. Van der Bruggen,
    Phys. Chem. Chem. Phys. 12 , 13333–13342 (2010).
    22. S. Darvishmaneshet al., Green Chem. 13 ,3476–3483 (2011).
    23. H. Siddiqueet al., Ind. Eng. Chem. Res. 52 ,1109– 1121
    (2013).
    24. H. Werhan, A. Farshori, P. Rudolf von Rohr,J. Membr. Sci.
    423-424, 404–412 (2012).
    25. R. Othman, A. W. Mohammad, M. Ismail, J. Salimon,
    J. Membr. Sci. 348 , 287–297 (2010).
    26. M. Morshed, H. Simonaire, H. Alem, D. Roizard,J. Appl.
    Polym. Sci. 137 , 48359 (2020).
    27. Z. F. Gao, G. M. Shi, Y. Cui, T.-S. Chung,J. Membr. Sci. 565 ,
    169 – 178 (2018).
    28. A. Asadi Tashvigh, L. Luo, T.-S. Chung, M. Weber, C. Maletzko,
    J. Membr. Sci. 551 , 204–213 (2018).
    29. M. F. Jimenez-Solomon, Q. Song, K. E. Jelfs, M. Munoz-Ibanez,
    A. G. Livingston,Nat. Mater. 15 , 760–767 (2016).
    30. S. Karan, Z. Jiang, A. G. Livingston,Science 348 ,1347–1351 (2015).
    31. J. H. Kimet al., J. Membr. Sci. 550 , 322–331 (2018).
    32. L. F. Villalobos, T. Huang, K. V. Peinemann,Adv. Mater. 29 ,
    1606641 (2017).
    33. J. Liu, D. Hua, Y. Zhang, S. Japip, T. S. Chung,Adv. Mater. 30 ,
    1705933 (2018).
    34. T. Huang, T. Puspasari, S. P. Nunes, K. V. Peinemann,
    Adv. Funct. Mater. 30 , 1906797 (2020).
    35. T. Huanget al., Nat. Commun. 11 , 5882 (2020).
    36. M. Amirilarganiet al., ChemSusChem 13 ,136–140 (2020).
    37. C. Liet al., J. Membr. Sci. 572 , 520–531 (2019).
    38. J. Liuet al., Sci. Adv. 6 , eabb1110 (2020).


ACKNOWLEDGMENTS
We thank V. Samaras (KAUST, Analytical Corelab) for the GCxGC
measurements, S. Aristizábal (KAUST) for valuable discussions,
and F. Alduraiei (KAUST) for providing the Arabian crude oil.
Funding:This work was sponsored by King Abdullah University of
Science and Technology (KAUST), Office of Vice President of
Research. The authors thank the Advanced Membranes and
Porous Materials (AMPM) Center for the CCF grant and general
discussions.Author contributions:Conceptualization: S.C., S.N.
Methodology and investigation: S.C. (design, membrane preparation,
SEM, separation performance), V.M. (mechanical properties, TEM,
DSC, rheology), G.F. (separation performance), W.Z. (FT-ICR MS and
GC-MS), E.A.H. (NMR), A.H.E. (EPR), M.A. (TGA-MS). Funding
acquisition and supervision: S.N. Writing–original draft: S.C., SN.
Writing–review and editing: S.C., S.N.Competing interests:The
authors declare no competing interests. S.C., V.M., and S.N. are
inventors on patent application US 63/174,376 recently submitted by
KAUST.Data and materials availability:All data are available in
the manuscript or the supplementary material.License information:
Copyright © 2022 the authors, some rights reserved; exclusive
licensee American Association for the Advancement of Science. No
claim to original US government works. https://www.science.org/
about/science-licenses-journal-article-reuse

SUPPLEMENTARY MATERIALS
science.org/doi/10.1126/science.abm7686
Materials and Methods
Figs. S1 to S25
Table S1
Submitted 10 October 2021; accepted 7 April 2022
10.1126/science.abm7686

Chiscaet al., Science 376 , 1105–1110 (2022) 3 June 2022 6of6


RESEARCH | REPORT

Free download pdf