Recent Progress in Enzyme Immobilization to Metal–Organic Frameworks to Enhance the CO2 Conversion Efficiency

Molecules, Journal Year: 2025, Volume and Issue: 30(2), P. 251 - 251

Published: Jan. 10, 2025

Climate change and the energy crisis, driven by excessive CO2 emissions, have emerged as pressing global challenges. The conversion of into high-value chemicals not only mitigates atmospheric levels but also optimizes carbon resource utilization. Enzyme-catalyzed technology offers a green efficient approach to conversion. However, free enzymes are prone inactivation denaturation under reaction conditions, which limit their practical applications. Metal-organic frameworks (MOFs) serve effective carriers for enzyme immobilization, offering porous crystalline structures that enhance stability. Moreover, high specific surface area facilitates strong gas adsorption, making enzyme@MOF composites particularly advantageous catalytic In this paper, we review synthesis technologies application enzyme@MOFs in Furthermore, strategies, including enhancement utilization, coenzyme regeneration efficiency, substrate mass transfer discussed further improve efficiency aim is present innovative ideas future research highlight potential applications achieving

Language: Английский

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Photoenzyme Coupling System: Covalent Organic Frameworks In Situ Production of Hydrogen Peroxide Cascaded with Unspecific Peroxygenase to Achieve C–H Bonds Selective Activation

ACS Applied Materials & Interfaces, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 15, 2025

As an efficient, sustainable, and environmentally friendly semiconductor material, covalent organic frameworks (COFs) can generate hydrogen peroxide (H2O2) by photocatalysis, attracting wide attention in recent years. Herein, the effects of hydroxyl, methoxyl, vinyl groups imide-linked two-dimensional (2D) COFs on photocatalytic production H2O2 were studied theoretically experimentally. The introduction greatly promotes photogenerated charge separation migration COFs, providing more oxygen adsorption sites, stronger proton affinity, lower intermediate binding energy, which effectively facilitates rapid conversion to H2O2. Further, we have integrated properties situ generation continuous consumption unspecific peroxygenases (UPOs) construct a mild simple photoenzyme coupling system that achieve selective activation C–H bonds without need any external oxidants or sacrificial agents. This simple, stable, compatible avoids irreversible enzyme damage caused excessive exogenous utilization agents, thus efficient green pathway for fine chemical synthesis. not only breaks restriction supplementation UPO catalytic but also provides new practical application direction production.

Language: Английский

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Rh-functionalized Imino-pyridine Covalent Organic Framework Assembled on Ti₃C₂T_x (MXene) for Efficient NADH Regeneration and Photoenzymatic CO₂ Reduction

ACS Sustainable Chemistry & Engineering, Journal Year: 2025, Volume and Issue: unknown

Published: March 4, 2025

Nicotinamide adenine dinucleotide (NADH) regeneration is crucial for sustainable enzymatic CO2 reduction. In this study, Ti3C2Tx (MXene) and [Cp*Rh(bpy)(H2O)]2+ (labeled as [Cp*Rh]) were sequentially assembled onto imino-pyridine structured covalent organic frameworks (TD-COF) to construct Rh@TDM photocatalysts with dual cocatalyst. The photoelectrochemical tests temperature-dependent photoluminescence spectra suggest that the synergistic effect of incorporation [Cp*Rh] immobilization enables a reduction in exciton binding energy promotes carrier transfer. Consequently, optimized [email protected] photocatalyst achieves 95.0% NADH yield, significantly higher than TD-COF free (32.7%). Additionally, modification strategy applied also enhances selectivity 1,4-NADH. Therefore, turnover frequency 1,4-NADH 1.06 h–1, which 7.1 times (0.15 h–1). Subsequently, photoenzymatic cascade catalytic system, obtained remarkable formate generation rate 2137.7 μmol g–1 h–1. This work not only provides novel example using COF containing an structure immobilize but reveals synergetic MXene facilitates These findings offer new insights opportunities design application artificial systems

Language: Английский

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Chemoenzymatic Sequential Catalysis with Carbonic Anhydrase for the Synthesis of Chiral Alcohols from Alkanes, Alkenes, and Alkynes

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(11), P. 8786 - 8793

Published: May 22, 2024

Chiral alcohols are important intermediates for various fine chemicals and pharmaceuticals. Integrating chemical catalysis efficient enzyme in sequential systems the synthesis of chiral is considered an ecofriendly promising approach. Herein, employing a highly selective carbonic anhydrase II different catalysts, we constructed three general chemoenzymatic alcohol compound from alkanes, alkenes, alkynes, respectively. Compared to classical approaches, combination promiscuous simple since it requires only mild reaction conditions avoids expensive ligands cumbersome operation steps. In this integrated approach, wide variety readily available aryl alkynes transformed into valuable with excellent enantioselectivity up 99% (nearly all above 90%). This unified strategy combining enzymatic catalyses advances process powerful transformations.

Language: Английский

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Rh-Functionalized Donor−π–Acceptor Covalent Organic Framework for Efficient Photocatalytic Nicotinamide Cofactor Regeneration

ACS Sustainable Chemistry & Engineering, Journal Year: 2024, Volume and Issue: 12(34), P. 12775 - 12785

Published: Aug. 12, 2024

A nicotinamide adenine dinucleotide phosphate (NADPH)-mediated photoenzyme-coupled catalytic system is an attractive and green strategy for chemical conversion. However, artificial photocatalytic NADPH regeneration with low activity selectivity has posed a challenge when it coupled enzyme catalysis. Therefore, we developed to prepare "all-in-one" photocatalyst (Rh-sp2c-COF) by immobilizing electron mediator ([Cp*Rh(bpy)(H2O)]2+) in covalent organic framework (COF) donor−π–acceptor structure efficient regeneration. The immobilized [Cp*Rh(bpy)(H2O)]2+ not only achieves specific of 1,4-NADPH but also improves the efficiency transfer utilization constructing intramolecular channels buffer tanks. In addition, expands range light absorption promotes effective carrier separation directional transfer. turnover frequency Rh-sp2c-COF reaches 2.17 mmol·gCOF–1·h–1, which 3.28, 1.99, 4.5 times higher than those sp2c-COF, sp2c-COF + free [Cp*Rh(bpy)(H2O)]2+, imine-COF, respectively. Finally, ene reductase asymmetric hydrogenation C═C. This work provides approach accurate predesign photocatalysts achieve conversion solar energy.

Language: Английский

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Multiple strategy for antibacterial effect via copper porphyrin doping polyphenolic aldehydes based covalent organic framework

Journal of environmental chemical engineering, Journal Year: 2024, Volume and Issue: 12(5), P. 113533 - 113533

Published: July 10, 2024

Language: Английский

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Electron-mediator-free efficient photocatalytic regeneration of coenzyme NAD(P)H via direct electron transfer using ultrathin Bi₂MoO₆ nanosheets

Green Chemistry, Journal Year: 2024, Volume and Issue: 27(3), P. 623 - 632

Published: Nov. 12, 2024

The direct electron transfer mechanism of single-layer Bi 2 MoO 6 ultrathin nanosheets promotes the efficient regeneration photocatalytic coenzyme NAD(P)H.

Language: Английский

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A Multiple Strategy for Antibacterial Effect Via Copper Porphyrin Doping Polyphenolic Aldehydes Based Covalent Organic Framework

Published: Jan. 1, 2024

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Language: Английский

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Development of Compatible Photocatalyst-Enzyme Hybrid System Via Intensifying Enzyme Tolerance for Enhanced Chiral Alcohol Synthesis

Published: Jan. 1, 2024

Language: Английский

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Development of compatible photocatalyst-enzyme hybrid system via Intensifying enzyme tolerance for enhanced chiral alcohol synthesis

Journal of Catalysis, Journal Year: 2024, Volume and Issue: unknown, P. 115932 - 115932

Published: Dec. 1, 2024

Language: Английский

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