Enzyme-mimicking of copper-sites in metal–organic frameworks for oxidative degradation of phenolic compounds

Valverde, Ainara; Alkain, Eneko; Rio-López, Natalia Ahiova; Lezama, Luis; Fidalgo-Marijuan, Arkaitz; Laza, José Manuel; Wuttke, Stefan; Porro, José María; Oyarzabal, Itziar; Jiménez-Ruiz, Mónica; García Sakai, Victoria; Arias, Pedro Luis; Agirrezabal-Telleria, Iker; Fernández de Luis, Roberto

doi:10.1039/d3ta06198a

J. Mater. Chem. A

2024

DOI: 10.1039/d3ta06198a

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Enzyme-mimicking of copper-sites in metal–organic frameworks for oxidative degradation of phenolic compounds

Ainara Valverde,

Eneko Alkain,

Natalia Ahiova Rio-López

et al.

Abstract: Two on the main factors that control the activity and selectivity of the metal sites within metalloenzymes are: (i) their coordination environments, and the (ii) number and connectivity of the...

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Cited by 4 publications

References 89 publications

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Metal‐Organic Frameworks for Dual Photo‐Oxidation and Capture of Arsenic from Water

G‐Saiz,

Gonzalez Navarrete,

Dutta

et al. 2024

ChemSusChem

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Despite rapid technological progress, heavy metal water pollution, particularly arsenic contamination, remains a significant global challenge. The stabilization of trivalent arsenic as neutral arsenite (AsIII) species hinders its removal by conventional adsorption methods. While adsorption of anionic arsenate (AsV) species is in principle more feasible, there are only a few adsorbents capable of adsorbing both forms of arsenic. In this work we study the potential of two well‐known families of Metal‐Organic Frameworks (MOFs), UiO‐66 and MIL‐125, to simultaneously adsorb and photo‐oxidize arsenic species from water. Our results demonstrate that the formation of AsV ions upon light irradiation promotes the subsequent adsorption of additional AsIII species. Thus, we propose the combined utilization of photocatalysis and adsorption technologies for water remediation purposes.

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Metal‐Organic Frameworks for Dual Photo‐Oxidation and Capture of Arsenic from Water

G‐Saiz,

Gonzalez Navarrete,

Dutta

et al. 2024

ChemSusChem

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A Host–Guest Approach to Engineering Oxidase-Mimetic Assembly with Substrate Selectivity and Dynamic Catalysis

Li,

Xie,

Zhang

et al. 2024

ACS Appl. Mater. Interfaces

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The creation of synthetic materials that emulate the complexity of natural systems, such as enzymes, remains a challenge in biomimicry. Here, we present a simple yet effective strategy to introduce substrate selectivity and dynamic responsiveness into an enzyme-mimetic supramolecular material. We achieved this by anchoring γ-cyclodextrin to a fluorene-modified Lys/Cu2+ assembly, which mimics copper-dependent oxidase. The binding affinity among the components was examined using 1H NMR, isothermal titration calorimetry (ITC), and theoretical simulation. The γ-cyclodextrin acts as a host, forming a complex with the fluorenyl moiety and aromatic substrates of specific sizes. This ensures the proximity of the substrate reactive groups to the copper center, leading to size-selective enhancement of aromatic substrate oxidation, particularly favoring biphenyl substrates. Notably, α- and β-cyclodextrins do not exhibit this effect, and the native oxidase lacks this selectivity. Additionally, the binding affinity of the aromatic substrate to the catalyst can be dynamically tuned by adding α-cyclodextrin or by irradiating with different wavelengths in the presence of competitive azo-guests, resulting in switched oxidative activities. This approach offers a new avenue for designing biomimetic materials with tailorable active site structures and catalytic properties.

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Mixed-valence metal–organic frameworks: concepts, opportunities, and prospects

Afshariazar,

Morsali

2025

Chem. Soc. Rev.

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Enzyme-mimicking of copper-sites in metal–organic frameworks for oxidative degradation of phenolic compounds

Abstract: Two on the main factors that control the activity and selectivity of the metal sites within metalloenzymes are: (i) their coordination environments, and the (ii) number and connectivity of the...

Cited by 4 publications

References 89 publications

Metal‐Organic Frameworks for Dual Photo‐Oxidation and Capture of Arsenic from Water

Metal‐Organic Frameworks for Dual Photo‐Oxidation and Capture of Arsenic from Water

A Host–Guest Approach to Engineering Oxidase-Mimetic Assembly with Substrate Selectivity and Dynamic Catalysis

Mixed-valence metal–organic frameworks: concepts, opportunities, and prospects

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