Hierarchical mesoporous metal–organic frameworks encapsulated enzymes: Progress and perspective

Zhang, Xueli; Tu, Rongxiu; Lü, Zan; Peng, Jinyun; Hou, Chaohuan; Wang, Zonghua

doi:10.1016/j.ccr.2021.214032

Cited by 74 publications

(39 citation statements)

References 119 publications

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“…The hierarchical ZIFs (HZIF) synthesis and enzyme postinfiltration to form BCL@HZIF were performed following literature procedure. − The PXRD and SEM images showed that the crystallinity and morphology were retained for mesoporous BCL@HZIFs (Figure S16 and S17). The size of intrinsic pores as measured in the pore-distribution analysis is about 1 nm, which is not big enough for enzyme adsorption.…”

Section: Methodsmentioning

confidence: 99%

Fine-Tuning the Micro-Environment to Optimize the Catalytic Activity of Enzymes Immobilized in Multivariate Metal–Organic Frameworks

Jian²,

Ren

et al. 2021

J. Am. Chem. Soc.

106

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The artificial engineering of an enzyme's structural conformation to enhance its activity is highly desired and challenging. Anisotropic reticular chemistry, best illustrated in the case of multivariate metal−organic frameworks (MTV-MOFs), provides a platform to modify a MOF's pore and inner-surface with functionality variations on frameworks to optimize the interior environment and to enhance the specifically targeted property. In this study, we altered the functionality and ratio of linkers in zeolitic imidazolate frameworks (ZIFs), a subclass of MOFs, with the MTV approach to demonstrate a strategy that allows us to optimize the activity of the encapsulated enzyme by continuously tuning the framework−enzyme interaction through the hydrophilicity change in the pores' microenvironment. To systematically study this interaction, we developed the component-adjustment-ternary plot (CAT) method to approach the optimal activity of the encapsulated enzyme BCL and revealed a nonlinear correlation, first incremental and then decremental, between the BCL activity and the hydrophilic linker' ratios in MTV-ZIF-8. These findings indicated there is a spatial arrangement of functional groups along the three-dimensional space across the ZIF-8 crystal with a unique sequence that could change the enzyme structure between closed-lid and open-lid conformations. These conformation changes were confirmed by FTIR spectra and fluorescence studies. The optimized BCL@ZIF-8 is not only thermally and chemically more stable than free BCL in solution, but also doubles the catalytic reactivity in the kinetic resolution reaction with 99% ee of the products.

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Section: Methodsmentioning

confidence: 99%

Fine-Tuning the Micro-Environment to Optimize the Catalytic Activity of Enzymes Immobilized in Multivariate Metal–Organic Frameworks

Jian²,

Ren

et al. 2021

J. Am. Chem. Soc.

106

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“…The application of MOFs combined with biocatalytic agents, including natural enzymes, is relatively recent. This integration has demonstrated an interesting synergistic performance in biocatalysis, due to the increased stability and reusability of encapsulated biocatalysts and the expansion of their applications into other fields [ 86 , 260 ]. Since the porosity properties of MOFs were identified, their investigation has developed exponentially [ 83 ].…”

Section: Future Trendsmentioning

confidence: 99%

The Chemistry and Applications of Metal–Organic Frameworks (MOFs) as Industrial Enzyme Immobilization Systems

et al. 2022

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Enzymatic biocatalysis is a sustainable technology. Enzymes are versatile and highly efficient biocatalysts, and have been widely employed due to their biodegradable nature. However, because the three-dimensional structure of these enzymes is predominantly maintained by weaker non-covalent interactions, external conditions, such as temperature and pH variations, as well as the presence of chemical compounds, can modify or even neutralize their biological activity. The enablement of this category of processes is the result of the several advances in the areas of molecular biology and biotechnology achieved over the past two decades. In this scenario, metal–organic frameworks (MOFs) are highlighted as efficient supports for enzyme immobilization. They can be used to ‘house’ a specific enzyme, providing it with protection from environmental influences. This review discusses MOFs as structures; emphasizes their synthesis strategies, properties, and applications; explores the existing methods of using immobilization processes of various enzymes; and lists their possible chemical modifications and combinations with other compounds to formulate the ideal supports for a given application.

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“…Metal–organic frameworks (MOFs), constructed by metal nodes and organic linkers, have 3D porous structures with very impressive characteristics, providing a kind of potential material for sensing applications. − From the beginning of this area, various MOF-based sensors have been extensively explored, including optical sensors and electrochemical sensors . Specifically, zirconium-porphyrin MOFs exhibit excellent water stability and unique chemical properties result from Zr nodes and porphyrin ligands, providing an ideal material for chemical sensing. , Recently, Zr-porphyrin MOF-based ratiometric fluorescent sensors have shown significant potential because of the unique porosity and structural tunability of the Zr-porphyrin MOF. − For these ratiometric fluorescent sensors, the built-in correction from different emission centers can dramatically improve the sensing performance.…”

Section: Introductionmentioning

confidence: 99%

Integration of Multiple Redox Centers into Porous Coordination Networks for Ratiometric Sensing of Dissolved Oxygen

Wang

Peng

et al. 2021

ACS Appl. Mater. Interfaces

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The application of porphyrin metal−organic frameworks (MOFs) as a ratiometric electrochemical sensing platform is still unexplored. In this paper, we report a ratiometric electrochemical sensor by the integration of multiple redox centers into porphyrin MOFs for the detection of dissolved oxygen (DO). Specifically, the ferrocene (Fc) group was integrated into the nanosized PCN-222(Fe) (PCN = porous coordination networks) via acid−base reaction to synthesize the Fc@PCN-222(Fe) composite with two redox centers of the Fc group and Fe-porphyrin. The Fc group that is insensitive to DO serves as an internal reference, and the Feporphyrin in PCN-222(Fe) is a DO indicator. The ratios of the cathodic currents for the two redox centers exhibit a linear relationship with DO concentrations from 2.8 to 28.9 mg mL −1 and a limit of detection of 0.3 mg mL −1 . In addition, the ratiometric electrochemical sensor has high selectivity and stability for DO sensing results from the Fc@PCN-222(Fe) composite. Because there are numerous redox centers, such as methylene blue and thionine, which can be integrated into MOFs, many MOF-based ratiometric electrochemical sensors can be simply developed for high-performance biosensing.

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Hierarchical mesoporous metal–organic frameworks encapsulated enzymes: Progress and perspective

Cited by 74 publications

References 119 publications

Fine-Tuning the Micro-Environment to Optimize the Catalytic Activity of Enzymes Immobilized in Multivariate Metal–Organic Frameworks

Fine-Tuning the Micro-Environment to Optimize the Catalytic Activity of Enzymes Immobilized in Multivariate Metal–Organic Frameworks

The Chemistry and Applications of Metal–Organic Frameworks (MOFs) as Industrial Enzyme Immobilization Systems

Integration of Multiple Redox Centers into Porous Coordination Networks for Ratiometric Sensing of Dissolved Oxygen

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