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Directed Assembly of Proteinaceous–Polysaccharide Nanofibrils to Fabricate Membranes for Emerging Contaminant Remediation

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Download Hi-Res ImageDownload to MS-PowerPointCite This:ACS Nano 2024, 18, 36, 25205-25215
    Article

    Directed Assembly of Proteinaceous–Polysaccharide Nanofibrils to Fabricate Membranes for Emerging Contaminant Remediation
    Click to copy article linkArticle link copied!

    • Yilin Zhang
      Yilin Zhang
      Department of Civil and Environmental Engineering, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, Massachusetts 02139, United States
      More by Yilin Zhang
      Orcidhttps://orcid.org/0000-0003-4246-3620
    • Hui Sun
      Hui Sun
      Department of Civil and Environmental Engineering, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, Massachusetts 02139, United States
      More by Hui Sun
      Orcidhttps://orcid.org/0000-0003-1831-2750
    • Yunteng Cao
      Yunteng Cao
      Department of Civil and Environmental Engineering, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, Massachusetts 02139, United States
      More by Yunteng Cao
      Orcidhttps://orcid.org/0000-0002-6425-7628
    • Maxwell J. Kalinowski
      Maxwell J. Kalinowski
      Department of Civil and Environmental Engineering, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, Massachusetts 02139, United States
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    • Meng Li
      Meng Li
      Department of Civil and Environmental Engineering, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, Massachusetts 02139, United States
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    • Benedetto Marelli*
      Benedetto Marelli
      Department of Civil and Environmental Engineering, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, Massachusetts 02139, United States
      *Email: [email protected]. Phone: (617) 253-7113.
      More by Benedetto Marelli
      Orcidhttps://orcid.org/0000-0001-5311-6961
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    ACS Nano

    Cite this: ACS Nano 2024, 18, 36, 25205–25215
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    https://doi.org/10.1021/acsnano.4c07409
    Published August 27, 2024
    Copyright © 2024 American Chemical Society
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    Abstract

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    Emerging contaminants, including per- and polyfluoroalkyl substances and heavy metals, are threatening the health of humans and ecosystems. Their removal from the environment remains challenging. Here, we designed silk fibroin–cellulose nanocrystal (silk-CNC) nanofibrillar and nanoporous membranes for emerging contaminant remediation. The protein–polysaccharide nanofibrils were fabricated by templating the assembly of silk fibroin using CNCs. Silk fibroin polymorphic nature combined with surface charge modulation of CNCs produced cationic silk-CNC(+) and anionic silk-CNC(−) nanofibrils that can target a broad spectrum of contaminants. Silk-CNC(+) nanofibrils and membranes exhibited antimicrobial properties and captured both short-chain heptafluorobutyric acid, perfluorobutanesulfonic acid, and long-chain perfluorooctanoic acid by virtue of hydrophobic attraction from β-sheeted silk fibroin and electrostatic interactions with CNC(+). Silk-CNC(−) provided the opportunity to target cations such as heavy metal cocontaminants. The nanofabrication of biopolymer-based membranes combines high performance with environmentally benign and cost-effective removal of emerging contaminants for water purification, wastewater treatment, and remediation.

    Copyright © 2024 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsnano.4c07409.

    • SFCNC elongation compressed (AVI)

    • Silk-CNC nanofibril formation at different silk-to-CNC mass ratios; CD spectra of silk, silk + CNC(–), and silk + CNC(+); porosity of silk-CNC membranes measured by mercury porosimeter; hardness and reduced modulus of silk and silk+CNC membranes measured by nanoindentation; stress–strain curves of silk-CNC membranes; cross section of a silk-CNC(+) membrane cast by 2 mL of 0.2 g L–1 silk-CNC nanofibril solutions; sorption capacities of CNC(+) and CNC(−); breakthrough curves of PFASs at 10 nmol concentration removed by silk-CNC(+) and silk-CNC(−) membranes; silk-CNC nanofibril formation at different silk concentrations, electrophoretic mobility, apparent zeta potential, and hydrodynamic diameter of CNC(+) and CNC(−); dimensions of CNC(−) and CNC(+) assessed by AFM; Young’s modulus of different silk-based nanomaterials; fitting parameters of PFAS sorption isotherms; PFAS sorption capacities of state-of-the-art sorbent materials; heavy metal sorption capacities of biopolymer-derived nanosorbent materials; fitting parameters of heavy metal sorption isotherms; summary of silk-based membrane materials for water purification; and concentration of PFBA, PFBS, and PFOA after filtered by 0.2 μm PES or cellulose acetate filters (PDF)

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    ACS Nano

    Cite this: ACS Nano 2024, 18, 36, 25205–25215
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsnano.4c07409
    Published August 27, 2024
    Copyright © 2024 American Chemical Society
    Request reuse permissions

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