4.8 Article

Incorporation of Cellulose Nanocrystals into Graphene Oxide Membranes for Efficient Antibiotic Removal at High Nutrient Recovery

Journal

ACS APPLIED MATERIALS & INTERFACES
Volume 13, Issue 12, Pages 14102-14111

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsami.0c20652

Keywords

two-dimensional (2D) materials; hybrid membrane; antibiotic removal; nutrient recovery; water separation

Funding

  1. United States Department of Agriculture [2018-68011-28371]

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In this study, a hybrid membrane of laminated graphene oxide and cellulose nanocrystals was fabricated to efficiently reject three typical antibiotics while allowing high passage of desirable nutrients. The research found that the removal mechanisms of different antibiotics vary, showing a certain degree of selectivity in the separation process.
Two-dimensional (2D) material-based membranes hold great promise in wastewater treatment. However, it remains challenging to achieve highly efficient and precise small molecule/ion separation with pure 2D material-fabricated lamellar membranes. In this work, laminated graphene oxide (GO)-cellulose nanocrystal (CNC) hybrid membranes (GO/CNC) were fabricated by taking advantages of the unique structures and synergistic effects generated from these two materials. The characterization results in physiochemical properties, and the structure of the as-synthesized hybrid membranes displayed enhanced membrane surface hydrophilicity, enhanced crumpling surface structure, and slightly enlarged interlayer-spacing with the incorporation of CNCs. Water permeability increases by two to four times with the addition of different CNC weight ratios in comparison to a pristine GO membrane. The optimal GO/CNC membrane achieved efficient rejection toward three typical antibiotics at 74.8, 90.9, and 97.2% for sulfamethoxazole (SMX), levofloxacin (Levo), and norfloxacin (Nor), respectively, while allowing a high passage of desirable nutrients such as NO3- and H2PO4-. It was found that SMX removal is primarily governed by electrostatic repulsion, while adsorption plays a crucial role in removing Levo and Nor. Moreover, the density functional theory calculations confirmed the increased antibiotic removal in the presence of an organic foulant, humic acid. Such a 2D material-based hybrid membrane offers a new strategy to develop fit-for purpose membranes for resource recovery and water separation.

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