Investigating the origin of high efficiency in confined multienzyme catalysis

Cao, Yufei; Li, Xiaoyang; Xiong, Jiarong; Wang, Licheng; Yan, Li‐Tang; Ge, Jun

doi:10.1039/c9nr07381g

Cited by 45 publications

(34 citation statements)

References 44 publications

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“…It is discovered that GOx@ZIF-8@HRP@ZIF-8 exhibited slightly decreased catalytic efficiency than GOx/HRP@ZIF-8 (Fig. 1k ), which is similar to previous work 71 , 72 that demonstrated close integration between GOx and HRP could facilitate in situ formed H 2 O 2 to immediately react with adjoining HRP, thus minimizing diffusion and self-decomposition of H 2 O 2 . Nevertheless, it is worth noting that GOx@ZIF-8@HRP@ZIF-8 still yielded 90.2% catalytic efficiency of GOx/HRP@ZIF-8, indicating that there is insignificant mass transport resistance cross over compartment boundaries within multi-shelled ZIF-8 41 .…”

Section: Resultssupporting

confidence: 88%

Hierarchically encapsulating enzymes with multi-shelled metal-organic frameworks for tandem biocatalytic reactions

et al. 2022

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Biocatalytic transformations in living organisms, such as multi-enzyme catalytic cascades, proceed in different cellular membrane-compartmentalized organelles with high efficiency. Nevertheless, it remains challenging to mimicking biocatalytic cascade processes in natural systems. Herein, we demonstrate that multi-shelled metal-organic frameworks (MOFs) can be used as a hierarchical scaffold to spatially organize enzymes on nanoscale to enhance cascade catalytic efficiency. Encapsulating multi-enzymes with multi-shelled MOFs by epitaxial shell-by-shell overgrowth leads to 5.8~13.5-fold enhancements in catalytic efficiencies compared with free enzymes in solution. Importantly, multi-shelled MOFs can act as a multi-spatial-compartmental nanoreactor that allows physically compartmentalize multiple enzymes in a single MOF nanoparticle for operating incompatible tandem biocatalytic reaction in one pot. Additionally, we use nanoscale Fourier transform infrared (nano-FTIR) spectroscopy to resolve nanoscale heterogeneity of vibrational activity associated to enzymes encapsulated in multi-shelled MOFs. Furthermore, multi-shelled MOFs enable facile control of multi-enzyme positions according to specific tandem reaction routes, in which close positioning of enzyme-1-loaded and enzyme-2-loaded shells along the inner-to-outer shells could effectively facilitate mass transportation to promote efficient tandem biocatalytic reaction. This work is anticipated to shed new light on designing efficient multi-enzyme catalytic cascades to encourage applications in many chemical and pharmaceutical industrial processes.

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Section: Resultssupporting

confidence: 88%

Hierarchically encapsulating enzymes with multi-shelled metal-organic frameworks for tandem biocatalytic reactions

et al. 2022

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“…However, the inactivation of enzyme is inevitable in the process of immobilization due to the change of enzyme structure, and the enhanced diffusion resistance between substrate and enzymes [20][21][22]. Recently, some novel methods for enzyme immobilization have been developed by co-precipitation of enzyme and inorganic components [23][24][25][26]. Especially, Ge et al developed an efficient method of enzyme immobilization, which called "enzymes-inorganic hybrid nanoflowers (HNF)" [27].…”

Section: Introductionmentioning

confidence: 99%

Bimetal based inorganic-carbonic anhydrase hybrid hydrogel membrane for CO2 capture

Wen

Zhang

et al. 2020

Journal of CO2 Utilization

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In this study, we synthesized for the first time a bimetal-based inorganic-carbonic anhydrase (CA) hybrid nanoflower to immobilize CA using Cu 2+ and Zn 2+ instead of single metal ion. Subsequently, the synthesized bimetallic hybrid nanoflowers (CANF) were embedded into the poly(vinyl alcohol) (PVA)-chitosan (CS) hydrogel networks to obtain PVA/CS@CANF hydrogel membrane. The CANF exhibited a significantly higher activity recovery of 70% compared with 35% with CA/Zn3(PO4)2 hybrid nanoflowers and 10% with CA/Cu3(PO4)2 hybrid nanoflowers. The PVA/CS@CANF hydrogel membrane possessed excellent mechanical strength, high catalytic activity, and were easy to flow out without centrifugation or filtration. At the same time, the PVA/CS@CANF displayed higher thermostability, storage stability, and pH stability than free CA and CANF, and superior reusability and CO2 capture capacity. The hydrogel membrane maintained more than 75% of its original activity after 8 cycles.However, CANF only maintained 12% of its original activity. Furthermore, the amount of CaCO3 produced by PVA/CS@CANF membrane was 9.0-fold and 2.0-fold compared with free CA and CANF, respectively. Therefore, This approach to synthesizing bimetallic-based protein hybrid hydrogel membrane could have a bright future in CO2 capture.

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“…210,214,[221][222][223][224] The benefits of the tightly-fitting ZIF are two-fold: the proximity of the enzyme to its container facilitates interactions that prevent enzyme leaching, and at high enough loadings, where mixtures of enzymes yield hetero-clusters, ZIF-encapsulation locks-in short separation distances between enzymes of differing identity -for example, sets of enzymes that can carry out successive stages of cascade reactions. 224,225 As noted by Ge et al, 225 close proximity of cascade actors can enable chemical intermediates to reach their destination and react before decaying. For diffusive transport, the required time increases as the square of the distance travelled.…”

Section: Enzymesmentioning

confidence: 96%

MOF-enabled confinement and related effects for chemical catalyst presentation and utilization

et al. 2022

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Investigating the origin of high efficiency in confined multienzyme catalysis

Abstract: Biomimetic strategies have successfully been applied to confine multiple enzymes on scaffolds to obtain higher catalytic efficiency of enzyme cascades than freely distributed enzymes.

Cited by 45 publications

References 44 publications

Hierarchically encapsulating enzymes with multi-shelled metal-organic frameworks for tandem biocatalytic reactions

Hierarchically encapsulating enzymes with multi-shelled metal-organic frameworks for tandem biocatalytic reactions

Bimetal based inorganic-carbonic anhydrase hybrid hydrogel membrane for CO2 capture

MOF-enabled confinement and related effects for chemical catalyst presentation and utilization

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