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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 | 2022 Jan

REPOSITORIES: biostudies-literature

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

Zhang Hao H Luo Jianquan J Wan Yinhua Y

iScience 20211222 1

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 increas ...[more]

PMID: 35028540

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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:Natural organic matter (NOM) present in surface water causes severe organic fouling of nanofiltration (NF) membranes employed for the production of potable water. Calcium (Ca2+) and magnesium (Mg2+) are alkaline earth metals present in natural surface water and severely exacerbate organic fouling owing to their ability to cause charge neutralization, complexation, and bridging of NOM and the membrane surface. Hence, it is of practical significance to engineer membranes with properties suitable for addressing organic fouling in the presence of these cations. This study employed OH-functionalized molybdenum disulphide (OH-MoS2) nanosheets as nanofillers via the interfacial polymerization reaction to engineer NF membranes for enhanced removal of NOM and fouling mitigation performance. At an optimized concentration of 0.010 wt.% of OH-MoS2 nanosheet, the membrane was endowed with higher hydrophilicity, negative charge and rougher membrane morphology which enhanced the pure water permeance by 46.33% from 11.2 to 16.39 L m-2 h-1 bar-1 while bridging the trade-off between permeance and salt selectivity. The fouling performance was evaluated using humic acid (HA) and sodium alginate (SA), which represent the hydrophobic and hydrophilic components of NOM in the presence of 0, 0.5, and 1 mM Ca2+ and Mg2+, respectively, and the performance was benchmarked with control and commercial membranes. The modified membrane exhibited normalized fluxes of 95.09% and 93.26% for HA and SA, respectively, at the end of the 6 h filtration experiments, compared to the control membrane at 89.71% and 74.25%, respectively. This study also revealed that Ca2+ has a more detrimental effect than Mg2+ on organic fouling and NOM removal. The engineered membrane outperformed the commercial and the pristine membranes during fouling tests in the presence of 1 mM Ca2+ and Mg2+ in the feed solution. In summary, this study has shown that incorporating OH-MoS2 nanosheets into membranes is a promising strategy for producing potable water from alternative water sources with high salt and NOM contents.

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

Publications

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

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