Hierarchically Porous Biocatalytic MOF Microreactor as a Versatile Platform towards Enhanced Multienzyme and Cofactor‐Dependent Biocatalysis

Angewandte Chemie International Edition, Journal Year: 2020, Volume and Issue: 60(10), P. 5421 - 5428

Published: Dec. 1, 2020

Metal-organic frameworks (MOFs) have recently emerged as excellent hosting matrices for enzyme immobilization, offering superior physical and chemical protection biocatalytic reactions. However, multienzyme cofactor-dependent biocatalysis, the subtle orchestration of enzymes cofactors is largely disrupted upon immobilizing in rigid crystalline MOF network, which leads to a much reduced efficiency. Herein, we constructed hierarchically porous MOFs by controlled structural etching enhance biocatalysis. The expanded size pores can provide sufficient space accommodated reorientate spread within their lower surface energy state well decrease inherent barriers accelerate diffusion rate reactants intermediates. Moreover, developed demonstrated outstanding tolerance inhospitable surroundings recyclability.

Language: Английский

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Insight of MOF Environment-Dependent Enzyme Activity via MOFs-in-Nanochannels Configuration

ACS Catalysis, Journal Year: 2020, Volume and Issue: 10(10), P. 5949 - 5958

Published: May 6, 2020

Maintaining the high activity of an enzyme is a fundamental requirement to widen application metal–organic frameworks (MOFs) in biotechnology, biosensor, and biomedicine fields. However, it still challenging monitor understand MOF environment-related for enzyme. Here, we developed MOFs-in-nanochannels configuration broadening biocatalytic MOFs on demand. ZIF-8 [Zn(mim)2, Hmim = 2-methylimidazolated] grown TiO2 nanochannels used as platform, cytochrome C (CytC) model encapsulated ZIF-8. The enzymatic catalytic process converts 2,2′-azino-bis(3-ethylbenzothiazoline-6-sulfonate) (ABTS) positively charged product (ABTS+). On basis current–voltage properties, change ion transport characteristics can be monitored with time. encapsulating CytC molecules not only exhibit significantly enhanced wide temperature region (37–80 °C) but also have remarkably long storage stability at room temperature. results quantum mechanical calculation indicate that Fe–S bond inclined break environment owing confinement effect structure, favorable catalysis. MOFs-in-nanochannel provides innovative label-free design onsite monitoring MOFs, which holds great potential constructing biosensing platforms remarkable performance stability.

Language: Английский

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Recent Trends in Enzyme Immobilization—Concepts for Expanding the Biocatalysis Toolbox

Molecules, Journal Year: 2021, Volume and Issue: 26(9), P. 2822 - 2822

Published: May 10, 2021

Enzymes have been exploited by humans for thousands of years in brewing and baking, but it is only recently that biocatalysis has become a mainstream technology synthesis. Today, enzymes are used extensively the manufacturing pharmaceuticals, food, fine chemicals, flavors, fragrances other products. Enzyme immobilization also developed parallel as means increasing enzyme performance reducing process costs. The aim this review to present discuss some more recent promising technical developments immobilization, including supports used, methods fabrication, their application highlights new support technologies such use well-established polysaccharides novel ways, magnetic particles, DNA, renewable materials hybrid organic–inorganic supports. addresses how being integrated into developing biocatalytic technology, example flow biocatalysis, 3D printing multi-enzymatic cascade reactions.

Language: Английский

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Insights into the Enhanced Catalytic Activity of Cytochrome c When Encapsulated in a Metal–Organic Framework

Journal of the American Chemical Society, Journal Year: 2020, Volume and Issue: 142(43), P. 18576 - 18582

Published: Oct. 13, 2020

The encapsulation of enzymes within porous materials has shown great promise, not only in protecting the from denaturation under nonbiological environments, but also, some cases, facilitating their enzymatic reaction rates at favorable conditions. While a number hypotheses have been developed to explain this phenomenon, detailed structural changes upon material, which are closely related activity, remain largely elusive. Herein, change cytochrome c (Cyt c) hierarchical metal-organic framework, NU-1000, is investigated through combination experimental and computational methods, such as electron paramagnetic resonance, solid-state ultraviolet-visible spectroscopy, all-atom explicit solvent molecular dynamics simulations. enhanced catalytic performance Cyt after being encapsulated NU-1000 supported by physical silico observations around heme ferric active center.

Language: Английский

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Hierarchical micro- and mesoporous ZIF-8 with core–shell superstructures using colloidal metal sulfates as soft templates for enzyme immobilization

Journal of Colloid and Interface Science, Journal Year: 2021, Volume and Issue: 610, P. 709 - 718

Published: Nov. 25, 2021

Language: Английский

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