Critical aspects of the stability and catalytic activity of MIL-100(Fe) in different advanced oxidation processes

Chávez, Ana M.; Rey, Ana; López, Jorge; Álvarez, Pedro M.; Beltrán, Fernando J.

doi:10.1016/j.seppur.2020.117660

Cited by 68 publications

(30 citation statements)

References 67 publications

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“…A typical example is given in Figure S7 , showing the formation of a new (large) band at around 1050 cm −1 , related to phosphate groups in the composition of the microMOFs upon their degradation in PBS. More specifically, this band corresponds to the asymmetrical P-O stretching [ 43 , 44 ]. Indeed, the degradation process follows a substitution mechanism.…”

Section: Resultsmentioning

confidence: 99%

Degradation Mechanism of Porous Metal-Organic Frameworks by In Situ Atomic Force Microscopy

Christodoulou

Bourguignon

et al. 2021

Nanomaterials

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In recent years, Metal-Organic Frameworks (MOFs) have attracted a growing interest for biomedical applications. The design of MOFs should take into consideration the subtle balance between stability and biodegradability. However, only few studies have focused on the MOFs’ stability in physiological media and their degradation mechanism. Here, we investigate the degradation of mesoporous iron (III) carboxylate MOFs, which are among the most employed MOFs for drug delivery, by a set of complementary methods. In situ AFM allowed monitoring with nanoscale resolution the morphological, dimensional, and mechanical properties of a series of MOFs in phosphate buffer saline and in real time. Depending on the synthetic route, the external surface presented either well-defined crystalline planes or initial defects, which influenced the degradation mechanism of the particles. Moreover, MOF stability was investigated under different pH conditions, from acidic to neutral. Interestingly, despite pronounced erosion, especially at neutral pH, the dimensions of the crystals were unchanged. It was revealed that the external surfaces of MOF crystals rapidly respond to in situ changes of the composition of the media they are in contact with. These observations are of a crucial importance for the design of nanosized MOFs for drug delivery applications.

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Section: Resultsmentioning

confidence: 99%

Degradation Mechanism of Porous Metal-Organic Frameworks by In Situ Atomic Force Microscopy

Christodoulou

Bourguignon

et al. 2021

Nanomaterials

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“…FTIR spectra of both MOFs are reported in Figure 2. They showed a broad absorption band at 3600-3000 cm -1 Wavenumber (cm [36,41,45], CH bending vibrations (~1112 cm -1 ) of the carboxylate groups in benzene rings [36,39,44], and CH vibrations (~760 and 708 cm -1 ) of these aromatic structures [46]. FTIR spectrum of MIL-101-Fe showed the absorption bands of asymmetric (~1590 cm -1 ) and symmetric (1390 cm -1 ) stretching vibration of the carboxyl groups (O-C=O) present in terephthalic acid, thus indicating the presence of the organic linker (i.e., dicarboxylate) in this sample [49,[51][52][53].…”

Section: Thermodynamics and Modeling Of The Adsorption Ofmentioning

confidence: 99%

Physicochemical Modeling of the Adsorption of Pharmaceuticals on MIL-100-Fe and MIL-101-Fe MOFs

Quintero-Álvarez

Rojas-Mayorga

Mendoza-Castillo

et al. 2022

Adsorption Science & Technology

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The adsorption of naproxen (NAP), diclofenac (DFC), and acetaminophen (APAP) molecules from aqueous solutions using MIL-100-Fe and MIL-101-Fe metal organic frameworks (MOFs) has been analyzed and modeled. Adsorption isotherms of these pharmaceuticals were experimentally quantified at 30 and 40°C and pH 7. Textural parameters and surface chemistry of these MOFs were analyzed, and results were utilized to explain the pharmaceutical adsorption mechanism. Density Functional Theory (DFT) calculations were performed to understand the reactivity of pharmaceutical molecules, and a statistical physics model was employed to calculate the main physicochemical parameters related to the adsorption mechanism. Results showed that the adsorption of these pharmaceuticals on MOFs was multimolecular and exothermic. Both MOFs displayed the highest adsorption capacities, up to 2.19 and 1.71 mmol/g, for NAP and DFC molecules, respectively. MIL-101-Fe showed better pharmaceutical adsorption properties than MIL-100-Fe due to its highest content of Fe-O clusters and mesopore volume. Adsorption mechanism of these organic molecules could involve hydrogen bond, van der Waals forces, and electrostatic interactions with MOF surfaces. In particular, MIL-101-Fe MOF is a promising material to prepare composites with competitive adsorption capacities for facing the water pollution caused by pharmaceutical compounds.

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“…Meanwhile, the surface areas of the hybrids were lower than that of MIL-100(Fe), which may be due to the presence of BiOCl or residual impurities such as traces of trimesic acid or to the inhibition of the formation of crystalline MIL-100(Fe). 35 The large surface area and proper aperture increased the potential of BiOCl/MIL-100(Fe) to interact with organic contaminants for catalytic degradation. The presence of mesopores favors multilight scattering/reflection, resulting in enhanced harvesting of the exciting light and thus improved photocatalytic activity.…”

Section: Resultsmentioning

confidence: 99%

“…Here, MIL-100(Fe) was synthesized following a previously reported sustainable method but with slight modication. 35,37 First, 0.912 g NaOH was dissolved in 48.6 mL water; then 1.676 g H 3 BTC was introduced into the aqueous NaOH, and the mixture was stirred at 65 C to obtain clear solution A. Subsequently, FeCl 2 $4H 2 O (1.44 g) solid was added into 48.6 mL water, and the mixture was stirred under totally enclosed conditions to obtain a green clear solution, denoted as solution B.…”

Section: Preparation Of Mil-100(fe)mentioning

confidence: 99%

“…Furthermore, MIL-100(Fe) with the chemical composition Fe 3 O(H 2 O) 2 (X)·{C 6 H 3 (COO) 3 } 2 · n H 2 O (X = OH − or F − ) ( n = 14.5) has excellent chemical stability and water stability and is relatively easy to synthesize. 35 In one study, the efficiency of heterogeneous Fenton processes based on the decomposition of H 2 O 2 over Fe clusters of MIL-100(Fe) to generate ˙OH was significantly enhanced under visible-light irradiation. 36 Nevertheless, almost all the reported hybrid materials composed of BiOX and Fe-MOFs were prepared via hydrothermal or solvothermal methods, or BiOX or Fe-MOFs were first prepared and then the composites were obtained.…”

Section: Introductionmentioning

confidence: 99%

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Highly efficient heterogeneous photo-Fenton BiOCl/MIL-100(Fe) nanoscaled hybrid catalysts prepared by green one-step coprecipitation for degradation of organic contaminants

Jiang

Tian

et al. 2021

RSC Adv.

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Critical aspects of the stability and catalytic activity of MIL-100(Fe) in different advanced oxidation processes

Cited by 68 publications

References 67 publications

Degradation Mechanism of Porous Metal-Organic Frameworks by In Situ Atomic Force Microscopy

Degradation Mechanism of Porous Metal-Organic Frameworks by In Situ Atomic Force Microscopy

Physicochemical Modeling of the Adsorption of Pharmaceuticals on MIL-100-Fe and MIL-101-Fe MOFs

Highly efficient heterogeneous photo-Fenton BiOCl/MIL-100(Fe) nanoscaled hybrid catalysts prepared by green one-step coprecipitation for degradation of organic contaminants

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