Degradation Mechanism of Metal–Organic Framework Drug Nanocarriers Studied by Solid-State Nuclear Magnetic Resonance and X-ray Absorption Near-Edge Structure Spectroscopy
In: ISSN: 0897-4756, 2022
Online
academicJournal
Zugriff:
International audience ; Metal–organic framework nanoparticles (nanoMOFs) are novel porous drug delivery systems whose features include high drug loading capacity, versatile functionalization, biocompatibility, and biodegradability. However, little knowledge about the nature of nanoMOF degradation mechanism is one of the many reasons that prevent their clinical use. MIL-100 (MIL stands for Matériaux de l’Institut Lavoisier) is among the most studied nanoMOFs for drug delivery. Here, we investigate at the atomic scale the degradation mechanism of metal(III)-trimesate nanoMIL-100 drug carrier in biological-mimicking phosphate medium. By using solid-state NMR (ssNMR) spectroscopy, we found that the first step of nanoMIL-100(Al) degradation is the substitution of labile water ligands, resulting in new coordination bonds between Al(III) and phosphate ions, followed by the substitution of trimesate ligands, leading to their release. The data indicated that the reaction-limiting step most likely is the formation of an inorganic aluminophosphate layer at the nanoparticle surface and that drug encapsulation and surface coating affect the nanoMIL-100(Al) degradation. The X-ray absorption near-edge structure (XANES) spectroscopy study of nanoMIL-100(Fe) degradation corroborates the hypothesized alteration mechanism of nanoMIL-100(Al). From the ensemble of data, a stepwise degradation mechanism representative for the nanoMIL-100 drug delivery system is proposed.
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Degradation Mechanism of Metal–Organic Framework Drug Nanocarriers Studied by Solid-State Nuclear Magnetic Resonance and X-ray Absorption Near-Edge Structure Spectroscopy
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Autor/in / Beteiligte Person: | Vuong, Dang Le Mai ; Christodoulou, Ioanna ; Porcino, Marianna ; Đồng, Sĩ Thành ; Lassalle-Kaiser, Benedikt ; Haouas, Mohamed ; Gref, Ruxandra ; Martineau-Corcos, Charlotte ; Institut Lavoisier de Versailles (ILV) ; Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Institut de Chimie - CNRS Chimie (INC-CNRS)-Centre National de la Recherche Scientifique (CNRS) ; Institut des Sciences Moléculaires d'Orsay (ISMO) ; Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS) ; Conditions Extrêmes et Matériaux : Haute Température et Irradiation (CEMHTI) ; Université d'Orléans (UO)-Institut de Chimie - CNRS Chimie (INC-CNRS)-Centre National de la Recherche Scientifique (CNRS) ; Synchrotron SOLEIL (SSOLEIL) ; Centre National de la Recherche Scientifique (CNRS) ; Financial support from the IR-RMN-THC Fr3050 CNRS for conducting the research is gratefully acknowledged. This work was also supported by the Paris Ile-de-France Région – DIM “Respore”. ; ANR-11-EQPX-0029,MORPHOSCOPE 2,Imagerie et reconstruction multiéchelles de la morphogenèse. (Plateforme d'innovation technologique et méthodologique pour l'imagerie in vivo et la reconstruction des dynamiques multiéchelles de la morphogenèse)(2011) ; ANR-10-INBS-0004,France-BioImaging,Développment d'une infrastructure française distribuée coordonnée(2010) ; ANR-11-IDEX-0003,IPS,Idex Paris-Saclay(2011) |
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Zeitschrift: | ISSN: 0897-4756, 2022 |
Veröffentlichung: | HAL CCSD ; American Chemical Society, 2022 |
Medientyp: | academicJournal |
DOI: | 10.1021/acs.chemmater.2c01190 |
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