Confining the motion of enzymes in nanofiltration membrane for efficient and stable removal of micropollutants

Zhang, Hao; Luo, Jianquan; Woodley, John M.; Wan, Yinhua

doi:10.1016/j.cej.2020.127870

Cited by 13 publications

(16 citation statements)

References 53 publications

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“…Laccase is mainly immobilized by the geometric confinement of the support layer of the NF membrane. Thereinto, PNIPAM modification can enhance the geometric confinement strength and specific surface area of the support layer, which benefits for enzyme immobilization and stabilization ( Zhang et al., 2020 ). Therefore, the enzyme loading of the PNIPAM-modified BNMs was much higher than that of the pristine-E ( Figure 5 B).…”

Section: Resultsmentioning

confidence: 99%

“…This can be explained by the fact that higher enzyme and microgels loading in the support layer induced higher steric hindrance, which severely hampered the accessibility of the substrate to laccase. Moreover, the high confinement strength of H-5wt%-E to laccase reduced the enzyme mobility and thus suppressed enzyme activity ( Zhang et al., 2020 ). In addition, the PNIPAM-based BNMs showed better operational stability than the pristine-E during four reuse cycles.…”

Section: Resultsmentioning

confidence: 99%

“…The hydrodynamic diameter of PNIPAM-PEI microgels at 25°C and 38°C was tested by DLS, which was 440 and 293 nm, respectively, exhibiting admirable temperature-responsive property ( Figure 10 C). Moreover, since PNIPAM-PEI microgels have a positive surface charge of 2.17 mV (due to the grafting of the cationic PEI chains) and the surface charge of laccase is −4.6 mV at pH 5 ( Zhang et al., 2020 ), laccase would be immobilized by electrostatic adsorption besides geometric confinement.

Figure 10 Synthesis and characterization of PNIPAM-PEI microgels (A) Scheme for the synthesis of PNIPAM-PEI microgels.…”

Section: Resultsmentioning

confidence: 99%

“…Thereinto, the enzyme loading of the pristine-E was the lowest, but its BPA removal efficiency in the first reuse cycle was higher than that of the PNIPAM-PEI-based BNMs ( Figure 11 F). This was because the high confinement strength of PNIPEM-PEI-based BNMs largely constricted the essential mobility of the immobilized laccase for efficient catalysis and thus led to a lower BPA removal efficiency ( Zhang et al., 2020 ). In contrast, the low enzyme mobility in PNIPEM-PEI-based BNMs significantly delayed the enzyme leakage, resulting in better reusability ( Figure 11 F).…”

Section: Resultsmentioning

confidence: 99%

“…Despite the low enzyme leakage by the above strategies, the high steric hindrance caused by PDA coating and nanomaterials led to a rigid structure of the immobilized enzyme and severe products accumulation, thereby reducing the enzyme activity and stability. Very recent findings by our group showed that rational design of the confinement strength of the support layer to the enzyme by polyelectrolytes-based three-dimensional modification method could improve the activity and stability of the BNMs ( Zhang et al., 2020 ). However, when the immobilized enzyme is inactivated or the OMPs removal efficiency cannot meet the demands, such BNMs are difficult to regenerate as the confinement strength of the membrane cannot be tuned once the membrane is fabricated.…”

Section: Introductionmentioning

confidence: 99%

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Regenerable temperature-responsive biocatalytic nanofiltration membrane for organic micropollutants removal

2022

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Summary 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.

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Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

Figure 10 Synthesis and characterization of PNIPAM-PEI microgels (A) Scheme for the synthesis of PNIPAM-PEI microgels.…”

Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Regenerable temperature-responsive biocatalytic nanofiltration membrane for organic micropollutants removal

2022

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3D Neighborhood Nanostructure Reinforces Biosensing Membrane

Song,

Zhang,

Wan

et al. 2023

Adv Funct Materials

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The electron signals in the cell can be rapidly and accurately transmitted by the spatially confined and adjacently distributed enzyme pairs anchored in the cytomembrane. As inspiration, by leverage of tannic acid‐3‐aminopropyltriethoxysilane‐Fe (TA‐APTES‐Fe) ternary coating, for the first time, a mesoporous biosensing membrane is developed by orderly assembly and targeted confinement of Prussian blue (PB) and glucose oxidase (GOx) with neighborhood nanostructure in the 3D mesoporous carbon nanotubes (CNTs) membrane electrode. The mesoporous biosensing membrane extends the triple‐phase boundary from conventional 2D contact to 3D contact, promotes the transfer rates of the cascade reactants, enhances the proximity of PB, GOx, and the electrode, and achieves in–situ removal of interferents, thereby elevating the utilization of PB, enhancing the cascade reaction efficiency, increasing the availability of the electroactive hydrogen peroxide (H2O2), and improving its stability. It exhibits superior sensitivity (31.2 µA mM−1) and long‐term stability in continuous glucose monitoring with a negligible response drift for up to 8 h. In addition, the multienzyme mimic functions of PB are employed to imitate the “loosening‐degradation” membrane cleaning process via bubble scrubbing and Fenton oxidation, thereby fully regenerating the fouled biosensing membrane. This work provides a novel design strategy for biosensors toward efficient, reliable, and stable sensing.

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Constructing biocatalytic nanochannel membranes for unidirectional isomer conversion and separation

et al. 2023

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Isomer conversion and separation are crucial in the chemical, pharmaceutical, and food industries. However, this process remains challenging due to the reversed conversion of isomers and their similar boiling points and kinetic diameters. Herein, an enzyme‐catalyzed nanochannel membrane with a hierarchical structure is fabricated for selective and directional isomeric conversion and separation. The enzyme is embedded in a confined polymer network that shows high stability and retains 95% of its initial activity after 50 reaction cycles. Studying the transport mechanisms between isomers through the membrane shows that the hierarchical layers of the membrane impose unequal energy barriers to the forward and backward transport of products, promoting unidirectional diffusion of products and interrupting the equilibrium of the isomerization reaction to increase the conversion rate by 43%. Overall, this work opens a new avenue for the design of biocatalytic nanochannel membranes and the directional production and in situ separation of isomers.

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Confining the motion of enzymes in nanofiltration membrane for efficient and stable removal of micropollutants

Cited by 13 publications

References 53 publications

Regenerable temperature-responsive biocatalytic nanofiltration membrane for organic micropollutants removal

Regenerable temperature-responsive biocatalytic nanofiltration membrane for organic micropollutants removal

3D Neighborhood Nanostructure Reinforces Biosensing Membrane

Constructing biocatalytic nanochannel membranes for unidirectional isomer conversion and separation

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