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Regenerable temperature-responsive biocatalytic nanofiltration membrane for organic micropollutants removal.

ABSTRACT: Biocatalytic nanofiltration membranes (BNMs) exhibit great potentials in organic micropollutants removal attributed to its synergistic effect between enzyme catalysis and membrane separation. However, the difficulties in regeneration of the BNMs halted their economic practicality. Inspired by cell membranes with stimuli-responsive channels, we have developed the temperature-responsive BNMs with nanogating function by poly(N-isopropyl acrylamide) (PNIPAM) modification. PNIPAM modification increases the geometric confinement of the support layer to enzymes, thus improving enzyme loading, inhibiting enzyme leakage, and preventing membrane permeability decline caused by enzyme excess migration and aggregation. By optimizing the concentration of reaction monomers, modification time, and strategies, the PNIPAM-based BNMs show high bisphenol A (BPA) removal efficiency and long-term stability. Furthermore, the PNIPAM-polyethyleneimine-based BNMs can be easily regenerated at 38°C, and the laccase activity and BPA removal efficiency are fully recovered. This work would promote the real application of BNMs in bioconversion, drug delivery, and biosensors.

SUBMITTER: Zhang H

PROVIDER: S-EPMC8741613 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:Water pollution by various toxic substances remains a serious environmental problem, especially the occurrence of organic micropollutants including endocrine disruptors, pharmaceutical pollutants and naphthol pollutants. Adsorption process has been an effective method for pollutant removal in wastewater treatment. However, the thermal regeneration process for the most widely used activated carbon is costly and energy-consuming. Therefore, there has been an increasing need to develop alternative low-cost and effective adsorption materials for pollutant removal. Herein, β-cyclodextrin (β-CD), a cheap and versatile material, was modified with methacrylate groups by reacting with methacryloyl chloride, giving an average degree of substitution of 3 per β-CD molecule. β-CD-methacrylate, which could function as a crosslinker, was then copolymerized with acrylamide monomer via free-radical copolymerization to form β-CD-polyacrylamide (β-CD-PAAm) hydrogel. Interestingly, in the structure of the β-CD-PAAm hydrogel, β-CD is not only a functional unit binding pollutant molecules through inclusion complexation, but also a structural unit crosslinking PAAm leading to the formation of the hydrogel 3D networks. Morphological studies showed that β-CD-PAAm gel had larger pore size than the control PAAm gel, which was synthesized using conventional crosslinker instead of β-CD-methacrylate. This was consistent with the higher swelling ratio of β-CD-PAAm gel than that of PAAm gel (29.4 vs. 12.7). In the kinetic adsorption studies, phenolphthalein, a model dye, and bisphenol A, propranolol hydrochloride, and 2-naphthol were used as model pollutants from different classes. The adsorption data for β-CD-PAAm gel fitted well into the pseudo-second-order model. In addition, the thermodynamic studies revealed that β-CD-PAAm gel was able to effectively adsorb the different dye and pollutants at various concentrations, while the control PAAm gel had very low adsorption, confirming that the pollutant removal was due to the inclusion complexation between β-CD units and pollutant molecules. The adsorption isotherms of the different dye and pollutants by the β-CD-PAAm gel fitted well into the Langmuir model. Furthermore, the β-CD-PAAm gel could be easily recycled by soaking in methanol and reused without compromising its performance for five consecutive adsorption/desorption cycles. Therefore, the β-CD-PAAm gel, which combines the advantage of an easy-to-handle hydrogel platform and the effectiveness of adsorption by β-CD units, could be a promising pollutant removal system for wastewater treatment applications.

Project description:Nowadays, public concern is focused on the degradation of water quality. For this reason, the development of innovative technologies for water treatment in view of (micro)pollutant removal is important. Indeed, organic (micro)pollutants, such as pharmaceuticals, herbicides, pesticides and plasticizers at concentration levels of μg L-1 or even ng L-1 are hardly removed during conventional wastewater treatment. In view of this, thermo-plasma expanded graphite, a light-weight innovative material in the form of a powder, was encapsulated into calcium alginate to obtain a granular form useful as filtration and adsorption material for removal of different pollutants. The produced material was used to remove atrazine, bisphenol-A, 17-α-ethinylestradiol and carbamazepine (at concentration levels of 125, 250 and 500 µg L-1) by top-down filtration. The effect of flow rate, bed depth and adsorbent composition was evaluated based on breakthrough curves. The experimental data was analysed with the Adams-Bohart model in view of scale-up. Under optimal conditions, removal and adsorption capacity of respectively about 21%, 21%, 38%,42%, 43 µg g-1, 44 µg g-1, 37 µg g-1 and 87 µg g-1 were obtained for atrazine, bisphenol, 17-α ethinylestradiol and carbamazepine when using 0.12 g of thermo-plasma expanded graphite to treat 200 mL at 500 µg L-1 (for each compound) of solution obtaining at contact time of 20 min. The granular form of TPEG obtained (GTPEG) by entrapping in calcium alginate results to have a good adsorbent property for the removal of carbamazepine, atrazine, bisphenol A and 17-α ethinylestradiol from water at concentration levels between 250 and 500 μg L-1. Promising results confirm the adsorbent properties of TPEG and push-up us to investigate on its application and improve of its performance by evaluating different entrapping materials.Supplementary informationThe online version contains supplementary material available at 10.1007/s40201-023-00876-9.

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Regenerable temperature-responsive biocatalytic nanofiltration membrane for organic micropollutants removal.

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