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Relating Selectivity and Separation Performance of Lamellar Two-Dimensional Molybdenum Disulfide (MoS2) Membranes to Nanosheet Stacking Behavior

  • Xinglin Lu*
    Xinglin Lu
    Department of Chemical and Environmental Engineering, Yale University, New Haven, Connecticut 06520-8286, United States
    *Phone: +1 203-444-3650; email: [email protected]
    More by Xinglin Lu
  • Uri R. Gabinet
    Uri R. Gabinet
    Department of Chemical and Environmental Engineering, Yale University, New Haven, Connecticut 06520-8286, United States
  • Cody L. Ritt
    Cody L. Ritt
    Department of Chemical and Environmental Engineering, Yale University, New Haven, Connecticut 06520-8286, United States
    More by Cody L. Ritt
  • Xunda Feng
    Xunda Feng
    Department of Chemical and Environmental Engineering, Yale University, New Haven, Connecticut 06520-8286, United States
    Center for Advanced Low-dimension Materials, State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, Donghua University, Shanghai 201620, China
    More by Xunda Feng
  • Akshay Deshmukh
    Akshay Deshmukh
    Department of Chemical and Environmental Engineering, Yale University, New Haven, Connecticut 06520-8286, United States
  • Kohsuke Kawabata
    Kohsuke Kawabata
    Department of Chemical and Environmental Engineering, Yale University, New Haven, Connecticut 06520-8286, United States
    Department of Chemistry, Graduate School of Science, Tohoku University, 6-3 Aoba, Aramaki, Aoba-Ku, Sendai, Miyagi 980-8578, Japan
  • Masashi Kaneda
    Masashi Kaneda
    Department of Chemical and Environmental Engineering, Yale University, New Haven, Connecticut 06520-8286, United States
  • Sara M. Hashmi
    Sara M. Hashmi
    Department of Chemical Engineering, Northeastern University, Boston, Massachusetts 02115-5000, United States
  • Chinedum O. Osuji
    Chinedum O. Osuji
    Department of Chemical and Environmental Engineering, Yale University, New Haven, Connecticut 06520-8286, United States
    Chemical and Biomolecular Engineering, University of Pennsylvania, Philadelphia, Pennsylvania 19104, United States
  • , and 
  • Menachem Elimelech*
    Menachem Elimelech
    Department of Chemical and Environmental Engineering, Yale University, New Haven, Connecticut 06520-8286, United States
    *Phone: +1 203-432-2789; email: [email protected]
Cite this: Environ. Sci. Technol. 2020, 54, 15, 9640–9651
Publication Date (Web):June 29, 2020
https://doi.org/10.1021/acs.est.0c02364
Copyright © 2020 American Chemical Society

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    Abstract

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    Increased demand for highly selective and energy-efficient separations processes has stimulated substantial interest in emerging two-dimensional (2D) nanomaterials as a potential platform for next-generation membranes. However, persistently poor separation performance continues to hinder the viability of many novel 2D-nanosheet membranes in desalination applications. In this study, we examine the role of the lamellar structure of 2D membranes on their performance. Using self-fabricated molybdenum disulfide (MoS2) membranes as a platform, we show that the separation layer of 2D nanosheet frameworks not only fails to demonstrate water-salt selectivity but also exhibits low rejection toward dye molecules. Moreover, the MoS2 membranes possess a molecular weight cutoff comparable to its underlying porous support, implying negligible selectivity of the MoS2 layer. By tuning the nanochannel size through intercalation with amphiphilic molecules and analyzing mass transport in the lamellar structure using Monte Carlo simulations, we reveal that small imperfections in the stacking of MoS2 nanosheets result in the formation of catastrophic microporous defects. These defects lead to a precipitous reduction in the selectivity of the lamellar structure by negating the interlayer sieving mechanism that prevents the passage of large penetrants. Notably, the imperfect stacking of nanosheets in the MoS2 membrane was further verified using 2D X-ray diffraction measurements. We conclude that developing a well-controlled fabrication process, in which the lamellar structure can be carefully tuned, is critical to achieving defect-free and highly selective 2D desalination membranes.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.est.0c02364.

    • Correlation of PEO molecular weight with hydrodynamic diameter (S1). Quantitative analysis of the orientational order of MoS2 nanosheets stacked in lamellar structures (S2). Determination of MoS2 Membrane packing density (S3). Determination of adsorption of dyes to membrane materials in filtration test (S4). Synthesis of MoS2 nanosheet suspension (Figure S1). Division of the size distribution of the synthesized MoS2 nanosheets into five equal bins for Monte Carlo simulation (Figure S2). Monte Carlo framework build-up with increasing film thickness (Figure S3). Representative AFM image and height profile of the synthesized MoS2 nanosheets (Figure S4). Molecular structure and space-filling model of dye molecules (Figure S5). Formation of dye aggregates in the aqueous phase (Figure S6). XRD patterns of an MoS2 membrane before and after PEO rejection test (Figure S7). Chemical structure of polyoxyethylene (20) cetyl ether (Brij58) (Figure S8). PEO rejection of the PVDF support, the MoS2 film, and the In-MoS2 film (Figure S9). Schematic illustration of the relationship between film thickness and interlayer spacing in a perfectly stacked film of MoS2 nanosheets (Figure S10). SEM cross-section images of the thick MoS2 films (Figure S11). Schematic illustration of possible effects of imperfect stacking of MoS2 nanosheet (Figure S12). Schematic illustration of the experimental setup of 1D XRD and 2D XRD measurements and their representative diffraction patterns (Figure S13). Schematic illustration of the MoS2 microdomain orientations (Figure S14). Schematic illustration of the 2D XRD instrument configurations (Figure S15). One-dimensional integrated data showing the plot of the intensity, I, vs the scattering vector, q, and the corresponding Gaussian fits (Figure S16). SEM cross-section micrographs of MoS2 membrane and MoS2 crystal (Figure S17). (PDF)

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