Peer-reviewed Publications |
Baczko, K., Fensterbank, H., Berini, B., Bordage, N., Clavier, G., Meallet-Renault, R., Larpent, C., & Allard, E. (2016). Azide-Functionalized Nanoparticles as Quantized Building Block for the Design of Soft-Soft Fluorescent Polystyrene Core-PAMAM Shell Nanostructures. Journal Of Polymer Science Part A-Polymer Chemistry, 54(1), 115–126.
Résumé: This work deals with the covalent coupling of azide-functionalized polymeric nanoparticles as a reactive core and amino-terminated PAMAM dendrons as a reactive shell. The nanoassemblies thereby obtained could be modified after the dendronization step by grafting an alkynyl Bodipy dye on the unreacted azide moieties. Only a few steps are required to attain nanoassemblies that could mimic dendrimers of high generation with sizes of nano-objects beyond those of dendrimers. The structure of the nanoassemblies are composed of a polystyrene core, an inner shell including the Bodipy dyes along with the internal branches of the PAMAM, and the terminal amino groups from the outer shell. The dendritic shell acts as a protective layer that prevents NP from aggregation in a surfactant free aqueous solution. The nano-objects display absorption and emission maxima above 500 nm with brightness that are the same order of magnitude than Qdots. (C) 2015 Wiley Periodicals, Inc.
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Boudjemaa, R., Briandet, R., Revest, M., Jacqueline, C., Caillon, J., Fontaine-Aupart, M. P., & Steenkeste, K. (2016). New Insight into Daptomycin Bioavailability and Localization in Staphylococcus aureus Biofilms by Dynamic Fluorescence Imaging. Antimicrobial Agents And Chemotherapy, 60(8), 4983–4990.
Résumé: Staphylococcus aureus is one of the most frequent pathogens responsible for biofilm-associated infections (BAI), and the choice of antibiotics to treat these infections remains a challenge for the medical community. In particular, daptomycin has been reported to fail against implant-associated S. aureus infections in clinical practice, while its association with rifampin remains a good candidate for BAI treatment. To improve our understanding of such resistance/ tolerance toward daptomycin, we took advantage of the dynamic fluorescence imaging tools (time-lapse imaging and fluorescence recovery after photobleaching [FRAP]) to locally and accurately assess the antibiotic diffusion reaction in methicillin-susceptible and methicillin-resistant S. aureus biofilms. To provide a realistic representation of daptomycin action, we optimized an in vitro model built on the basis of our recently published in vivo mouse model of prosthetic vascular graft infections. We demonstrated that at therapeutic concentrations, daptomycin was inefficient in eradicating biofilms, while the matrix was not a shield to antibiotic diffusion and to its interaction with its bacterial target. In the presence of rifampin, daptomycin was still present in the vicinity of the bacterial cells, allowing prevention of the emergence of rifampin-resistant mutants. Conclusions derived from this study strongly suggest that S. aureus biofilm resistance/ tolerance toward daptomycin may be more likely to be related to a physiological change involving structural modifications of the membrane, which is a strain-dependent process.
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Chagas, G. R., Xie, X., Darmanin, T., Steenkeste, K., Gaucher, A., Prim, D., Meallet-Renault, R., Godeau, G., Amigoni, S., & Guittard, F. (2016). Electrodeposition of Polypyrenes with Tunable Hydrophobicity, Water Adhesion, and Fluorescence Properties. Journal Of Physical Chemistry C, 120(13), 7077–7087.
Résumé: The control in surface hydrophobicity and water adhesion is extremely important for various applications in water harvesting, oil/water separation membrane, energy systems or biosensing, for example. Here, for the first time we show that the use of fluorescent monomers such as pyrene with various substituents differing by their hydrophobicity, size, or rigidity/flexibility can lead to surfaces with tunable hydrophobicity, water adhesion and fluorescence properties by a direct electropolymerization process. Seven original monomers with fluoroalkyl, alkyl, phenyl, adamantyl, and triethylene glycol substituents were synthesized and studied. The surface roughness is highly dependent on the substituent, and it seems that the fluorescence, although complex, correlates with the surface roughness. Superhydrophobic properties and highly oleophobic properties are obtained using fluoroalkyl chains due to the presence of nanostructured microparticles. In comparison to the structured absorption and emission bands of pyrene monomers, the pyrene polymers (oligomers) exhibit a broad structureless spectral shape both in absorption and in emission, which seems to be due to pyrene oligomerization and aggregation. This work is a first tentative attempt to combine superhydrophobic and fluorescent properties using an innovative strategy and opens new doors to explore in this domain.
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Conte, C., Fotticchia, I., Tirino, P., Moret, F., Pagano, B., Gref, R., Ungaro, F., Reddi, E., Giancola, C., & Quaglia, F. (2016). Cyclodextrin-assisted assembly of PEGylated polyester nanoparticles decorated with folate. Colloids And Surfaces B-Biointerfaces, 141, 148–157.
Résumé: In the last decades, nano-oncologicals bearing a polyethylene glycol (PEG) coating are being emerging as biomimetic devices able to drive their drug cargo to solid tumors through passive mechanisms. To improve selectivity toward cancer cells, nanocarriers decorated with the small ligand folate have been widely investigated. Nevertheless, a great challenge remains the effective exposition of folate on nanoparticles (NPs), which is a key prerequisite to ensure the correct binding to receptor and the following endocytic uptake. On these premises, in this study we propose a novel strategy to produce core-shell folate-targeted NPs based on diblock copolymers of poly(epsilon-caprolactone) (PCL) and PEG through the aid of (2-hydroxypropyl)-beta-cyclodextrin (HPPCD). PCL4300-PEG(2000) and PCL4300-PEG(2000)-Fol copolymers were synthesized, characterized and employed to produce NPs without and with HP beta CD by a melting/sonication procedure. Colloidal properties of targeted NPs produced with HP beta CD demonstrated a highly extended conformation of PEG chains in the shell, an enhanced interaction with a specific antibody against folate and a higher uptake in cells overexpressing folate receptor. Overall, these results suggest that proper manipulation of PEG shell conformation through HP beta CD can represent a novel non-covalent strategy to modify shell features. (C) 2016 Elsevier B.V. All rights reserved.
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Ding, J. X., Cheng, Y. L., Li, M. Q., Gref, R., & Chen, X. S. (2016). Smart Polymeric Nanocarriers. Journal Of Nanomaterials, .
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Duchene, D., & Gref, R. (2016). Small is beautiful: Surprising nanoparticles. International Journal Of Pharmaceutics, 502(1-2), 219–231.
Résumé: In the preparation of nanoparticles for drug delivery, it is well known that their size as well as their surface decorations can play a major role in interaction with living media. It is less known that their shape and internal structure can interplay with cellular and in vivo fate. The scientific literature is full of a large variety of surprising terms referring to their shape and structure. The aim of this review is to present some examples of the most often encountered surprising nanoparticles prepared and usable in the pharmaceutical technology domain. They are presented in two main groups related to their physical aspects: 1) smooth surface particles, such as Janus particles, “snowmen”, “dumbbells”, “rattles”, and “onions” and 2) branched particles, such as “flowers”, “stars” and “urchins”. The mode of preparation and potential applications are briefly presented. The topic has a serious, wider importance, namely in opportunity these structures have to allow exploration of the role of shape and structure on the utility (and perhaps toxicity) of these nanostructures. (C) 2016 Elsevier B.V. All rights reserved.
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Duchene, D., Cavalli, R., & Gref, R. (2016). Cyclodextrin-based Polymeric Nanoparticles as Efficient Carriers for Anticancer Drugs. Current Pharmaceutical Biotechnology, 17(3), 248–255.
Résumé: Among the difficulties encountered in the treatment of cancer are the physico-chemical properties of the chemotherapeutic agents; in particular low water solubility and low stability, resulting in poor efficacy. Due to their capability to form molecular inclusions with apolar molecules (or part of them) cyclodextrins constitute a powerful tool to prepare more efficient chemotherapeutic delivery systems such as nanoparticles. This review focuses on polymeric nanoparticles for cancer therapy prepared from either cyclodextrin molecules, or polymer and cyclodextrins.
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Fensterbank, H., Baczko, K., Constant, C., Idttalbe, N., Bourdreux, F., Vallee, A., Goncalves, A. M., Meallet-Renault, R., Clavier, G., Wright, K., & Allard, E. (2016). Sequential Copper-Catalyzed Alkyne-Azide Cycloaddition and Thiol-Maleimide Addition for the Synthesis of Photo- and/or Electroactive Fullerodendrimers and Cysteine-Functionalized Fullerene Derivatives. Journal Of Organic Chemistry, 81(18), 8222–8233.
Résumé: In this study, the functionalization of a fullerene building block in a stepwise process by means of the copper- catalyzed alkyne azide cycloaddition (CuAAC) and thiol- maleimide reactions is reported. Grafting of the fullerene plat- form with a variety of azido derivatives, including Bodipy, pyrene and ferrocene, was carried out first. These fullerene compounds were then reacted with thiol derivatives to yield sophisticated structures comprising photo- and/or electroactive fullerodendrimers and cysteine-functionalized fullerene assemblies. This strategy, which combines the CuAAC and thiol-maleimide processes, could become more widely adopted in the field of fullerene chemistry.
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Grazon, C., Rieger, J., Beaunier, P., Meallet-Renault, R., & Clavier, G. (2016). Fluorescent core-shell nanoparticles and nanocapsules using comb-like macromolecular RAFT agents: synthesis and functionalization thereof. Polymer Chemistry, 7(25), 4272–4283.
Résumé: Fluorescent nanoparticles and nanocapsules (FNPs) were synthesized via a one-pot RAFT miniemulsion process copolymerizing BODIPY-methacrylate and styrene in water. Ultra-bright sub-100 nm core-shell nanoparticles could be obtained with BODIPY covalently linked in the core, and possessing various shells. The nature and architecture of the particle shells could be tuned by using different macromolecular RAFT (macro-RAFT) agents in the miniemulsion polymerization process. The macro-RAFT agents were composed of poly(ethylene oxide) acrylate (PEOA) and/or acrylic acid (AA), owing to their biocompatibility and functionality respectively, in different proportions. Interestingly, with comb-like macro-RAFT agents comprising a high number of PEOA, nanocapsules were formed, while with linear macro-RAFT agents or with those exhibiting a high number of AA, full core-shell nanoparticles were obtained. For all the structures the control over the polymerization, the size, morphology, and zeta-potential as well as the photophysical properties were measured and compared with FNPs exhibiting a linear PEO-b-PAA block copolymer shell structure (C. Grazon, J. Rieger, R. Mallet-Renault, G. Clavier and B. Charleux, Macromol. Rapid Commun., 2011, 32, 699). Regardless of the shell structures, the brightness of the formed nanoparticles was estimated to be 100-1000 times higher than that of quantum dots. Ultimately, the shell of the different FNPs was functionalized with a second fluorophore via the AA's carboxyl groups. Thus, watersoluble ultra-bright FNPs with two fluorophores in distinct environments (water and in polystyrene) were obtained. They should have great potential for bioimaging applications.
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Izumi, Y., Fujii, K., Wien, F., Houee-Levin, C., Lacombe, S., Salado-Leza, D., Porcel, E., Masoud, R., Yamamoto, S., Refregiers, M., du Penhoat, M. A. H., & Yokoya, A. (2016). Structure Change from beta-Strand and Turn to alpha-Helix in Histone H2A-H2B Induced by DNA Damage Response. Biophysical Journal, 111(1), 69–78.
Résumé: Using synchrotron radiation-based circular dichroism spectroscopy, we found that the DNA damage response induces an increase of alpha-helix structure and a decrease of beta-strand and turn structures in histone H2A-H2B extracted from x-irradiated human HeLa cells. The structural alterations correspond to the assumption that an average of eight amino acid residues form new alpha-helix structures at 310 K. We propose the structural transition from beta-strand and turn structures to an a-helix structure in H2A-H2B as a novel, to our knowledge, process involved in the DNA damage response.
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Liu, B. T., Li, H. Y., Xu, X. N., Li, X., Lv, N. N., Singh, V., Stoddart, J. F., York, P., Xu, X., Gref, R., & Zhang, J. W. (2016). Optimized synthesis and crystalline stability of gamma-cyclodextrin metal-organic frameworks for drug adsorption. International Journal Of Pharmaceutics, 514(1), 212–219.
Résumé: The biocompatible and renewable cyclodextrin metal-organic frameworks (CD-MOFs) have addressed a range of opportunities in molecular storage and separation sciences. The reported protocols for their synthesis, however, were carried out at room temperature over long time periods of time (24 h), producing crystals of relatively poor uniformity. In this investigation, micron sized gamma-CD-MOFs were synthesized by an optimized vapor diffusion method at elevated temperature (50 degrees C) within 6 h, after which the size control, crystalline stability and drug adsorption behavior were investigated in detail. In this manner, uniform cubic gamma-CD-MOF crystals were obtained when the reaction temperature was raised to 50 degrees C with pre-addition of the reaction solvent. The size of gamma-CD-MOFs was adjusted efficiently by changing the reactant concentrations, temperatures, time, gamma-CD ratios to KOH and surfactant concentrations, without influencing the porosity and crystallinity of the material markedly. Varing degrees of reduction in crystallinity and change in morphology were observed when the gamma-CD-MOF crystals are treated under conditions of high temperature (100 degrees C), high humidity (92.5%) and polar solvents (e.g., MeOH and DMF). In relation to drug adsorption by gamma-CD-MOFs, most of the drug molecules containing carboxyl groups showed relatively high adsorption (> 5%), while low adsorption (< 5%) was found for drugs with nitrogen-containing heterocyclic rings. In addition, the adsorption kinetics of captopril to standard gamma-CD-MOFs matched a pseudo-second-order model rather well, whilst captopril adsorption to the damaged gamma-CD-MOFs only partially matched the pseudo-second-order model. In summary, based upon the optimized synthesis and size control of gamma-CD-MOFs, the crystalline stability and drug adsorption characteristics of gamma-CD-MOF crystals have been evaluated as a fundamental requirement of a potential vehicle for drug delivery. (C) 2016 Elsevier B.V. All rights reserved.
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Revest, M., Jacqueline, C., Boudjemaa, R., Caillon, J., Le Mabecque, V., Breteche, A., Steenkeste, K., Tattevin, P., Potel, G., Michelet, C., Fontaine-Aupart, M. P., & Boutoille, D. (2016). New in vitro and in vivo models to evaluate antibiotic efficacy in Staphylococcus aureus prosthetic vascular graft infection. Journal Of Antimicrobial Chemotherapy, 71(5), 1291–1299.
Résumé: Prosthetic vascular graft infection (PVGI) is an emerging disease, mostly caused by staphylococci, with limited data regarding efficacy of current antistaphylococcal agents. We aimed to assess the efficacy of different antibiotic regimens. Six different strains of MSSA and MRSA were used. We compared results of minimal biofilm inhibitory and eradicating concentrations (MBICs and MBECs) obtained with a Calgary Biofilm Pin Lid Device (CBPD) with those yielded by an original Dacron (R)-related minimal inhibitory and eradicating concentration measure model. We then used a murine model of Staphylococcus aureus vascular prosthetic material infection to evaluate efficacy of different antibiotic regimens: vancomycin and daptomycin combined or not with rifampicin for MRSA and the same groups with cloxacillin and cloxacillin combined with rifampicin for MSSA. We demonstrated that classical measures of MBICs and MBECs obtained with a CPBD could overestimate the decrease in antibiotic susceptibility in material-related infections and that the nature of the support used might influence the measure of biofilm susceptibility, since results yielded by our Dacron (R)-related minimal eradicating assay were lower than those found with a plastic device. In our in vivo model, we showed that daptomycin was significantly more bactericidal than comparators for some strains of MRSA or MSSA but not for all. For the majority of strains, it was as efficient as comparators. The addition of rifampicin to daptomycin did not enhance daptomycin efficacy. Despite the heterogeneity of results according to bacterial strains, these innovative models represent an option to better evaluate the in vitro efficacy of antibiotics on Dacron (R)-related biofilm S. aureus infections, and to screen different antibiotic regimens in a mouse model of PVGIs.
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Schlatholter, T., Eustache, P., Porcel, E., Salado, D., Stefancikova, L., Tillement, O., Lux, F., Mowat, P., Biegun, A. K., van Goethem, M. J., Remita, H., & Lacombe, S. (2016). Improving proton therapy by metal-containing nanoparticles: nanoscale insights. International Journal Of Nanomedicine, 11, 1549–1556.
Résumé: The use of nanoparticles to enhance the effect of radiation-based cancer treatments is a growing field of study and recently, even nanoparticle-induced improvement of proton therapy performance has been investigated. Aiming at a clinical implementation of this approach, it is essential to characterize the mechanisms underlying the synergistic effects of nanoparticles combined with proton irradiation. In this study, we investigated the effect of platinum- and gadolinium-based nanoparticles on the nanoscale damage induced by a proton beam of therapeutically relevant energy (150 MeV) using plasmid DNA molecular probe. Two conditions of irradiation (0.44 and 3.6 keV/mu m) were considered to mimic the beam properties at the entrance and at the end of the proton track. We demonstrate that the two metal-containing nanoparticles amplify, in particular, the induction of nanosize damages (>2 nm) which are most lethal for cells. More importantly, this effect is even more pronounced at the end of the proton track. This work gives a new insight into the underlying mechanisms on the nanoscale and indicates that the addition of metal-based nanoparticles is a promising strategy not only to increase the cell killing action of fast protons, but also to improve tumor targeting.
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Si, Y., Grazon, C., Clavier, G., Rieger, J., Audibert, J. F., Sclavi, B., & Meallet-Renault, R. (2016). Rapid and accurate detection of Escherichia coli growth by fluorescent pH-sensitive organic nanoparticles for high-throughput screening applications. Biosensors & Bioelectronics, 75, 320–327.
Résumé: Rapid detection of bacterial growth is an important issue in the food industry and for medical research. Here we present a novel kind of pH-sensitive fluorescent nanoparticles (FANPs) that can be used for the rapid and accurate real-time detection of Escherichia coil growth. These organic particles are designed to be non-toxic and highly water-soluble. Here we show that the coupling of pH sensitive fluoresceinamine to the nanoparticles results in an increased sensitivity to changes in pH within a physiologically relevant range that can be used to monitor the presence of live bacteria. In addition, these FANPs do not influence bacterial growth and are stable over several hours in a complex medium and in the presence of bacteria. The use of these FANPs allows for continuous monitoring of bacterial growth via real-time detection over long time scales in small volumes and can thus be used for the screening of a large number of samples for high-throughput applications such as screening for the presence of antibiotic resistant strains. (C) 2015 Elsevier B.V. All rights reserved.
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Simon-Yarza, M. T., Baati, T., Paci, A., Lesueur, L. L., Seck, A., Chiper, M., Gref, R., Serre, C., Couvreur, P., & Horcajada, P. (2016). Antineoplastic busulfan encapsulated in a metal organic framework nanocarrier: first in vivo results. Journal Of Materials Chemistry B, 4(4), 585–588.
Résumé: Nanoparticles of a mesoporous iron(III) trimesate MIL-100 nanocarrier encapsulating high amounts of the challenging antineoplastic busulfan were administered to rats and compared with the commercial Busilvex (R). Large differences in serum concentration of both busulfan and trimesate revealed the great impact of drug encapsulation both on the drug and on nanoparticle pharmacokinetics during the first 24 h of administration.
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Simon-Yarza, T., Baati, T., Neffati, F., Njim, L., Couvreur, P., Serre, C., Gref, R., Najjar, M. F., Zakhama, A., & Horcajada, P. (2016). In vivo behavior of MIL-100 nanoparticles at early times after intravenous administration. International Journal Of Pharmaceutics, 511(2), 1042–1047.
Résumé: Metal-organic frameworks have shown interesting features for biomedical applications, such as drug delivery and imaging agents. The benchmarked mesoporous iron(III) trimesate MIL-100 MOF nanocarrier combines progressive release of high drug cargoes with absence of visible in vivo toxicity. Although in a previous study pharmacokinetics and biodistribution of MIL-100 nanoparticles were evaluated in the long term (from 24h to 1 month), the crucial times for drug targeting and delivery applications are shorter (up to 24 h). Thus, this work aims to study the blood circulating profile and organ accumulation of MIL-100 nanocarrier at early times after administration. For this purpose, after intravenous administration to rats, both constitutive components of MIL-100 (trimesate and iron) were quantified by high performance liquid chromatography and a spectrophotometric method, respectively. The pharmacokinetic profile suggested that the nanoparticles act as a depot in the blood stream during the first hours before being cleared. Accumulation took mainly place in the liver and, in some extent, in the spleen. Nevertheless, histological studies demonstrated the absence of morphological alterations due to the presence of the particles in these organs. Liver function was however slightly altered as reflected by the increased plasma aspartate aminotransferase concentrations. Finally trimesate was progressively eliminated in urine. (C) 2016 Elsevier B.V. All rights reserved.
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Stefancikova, L., Lacombe, S., Salado, D., Porcel, E., Pagacova, E., Tillement, O., Lux, F., Depes, D., Kozubek, S., & Falk, M. (2016). Effect of gadolinium-based nanoparticles on nuclear DNA damage and repair in glioblastoma tumor cells. Journal Of Nanobiotechnology, 14.
Résumé: Background: Tumor targeting of radiotherapy represents a great challenge. The addition of multimodal nanoparticles, such as 3 nm gadolinium-based nanoparticles (GdBNs), has been proposed as a promising strategy to amplify the effects of radiation in tumors and improve diagnostics using the same agents. This singular property named theranostic is a unique advantage of GdBNs. It has been established that the amplification of radiation effects by GdBNs appears due to fast electronic processes. However, the influence of these nanoparticles on cells is not yet understood. In particular, it remains dubious how nanoparticles activated by ionizing radiation interact with cells and their constituents. A crucial question remains open of whether damage to the nucleus is necessary for the radiosensitization exerted by GdBNs (and other nanoparticles). Methods: We studied the effect of GdBNs on the induction and repair of DNA double-strand breaks (DSBs) in the nuclear DNA of U87 tumor cells irradiated with.-rays. For this purpose, we used currently the most sensitive method of DSBs detection based on high-resolution confocal fluorescence microscopy coupled with immunodetection of two independent DSBs markers. Results: We show that, in the conditions where GdBNs amplify radiation effects, they remain localized in the cytoplasm, i.e. do not penetrate into the nucleus. In addition, the presence of GdBNs in the cytoplasm neither increases induction of DSBs by.-rays in the nuclear DNA nor affects their consequent repair. Conclusions: Our results suggest that the radiosensitization mediated by GdBNs is a cytoplasmic event that is independent of the nuclear DNA breakage, a phenomenon commonly accepted as the explanation of biological radiation effects. Considering our earlier recognized colocalization of GdBNs with the lysosomes and endosomes, we revolutionary hypothesize here about these organelles as potential targets for (some) nanoparticles. If confirmed, this finding of cytoplasmically determined radiosensitization opens new perspectives of using nano-radioenhancers to improve radiotherapy without escalating the risk of pathologies related to genetic damage.
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Vu, T. T., Meallet-Renault, R., Clavier, G., Trofimov, B. A., & Kuimova, M. K. (2016). Tuning BODIPY molecular rotors into the red: sensitivity to viscosity vs. temperature. Journal Of Materials Chemistry C, 4(14), 2828–2833.
Résumé: Viscosity variations in the microscopic world are of paramount importance for diffusion and reactions. In the last decade a new class of fluorescent probes for measuring viscosity has emerged termed 'molecular rotors', which allows quantitative mapping of viscosity in microscopically heterogeneous environments. Here we attempt to tune the absorption and emission of one such 'molecular rotor' based on the BODIPY fluorescent core into the red region of the spectrum, to allow better compatibility with the 'tissue optical window' and imaging of cells and tissues. We consequently find that our redemitting BODIPY fluorophores are sensitive to environmental temperature rather than to viscosity, thus suggesting a new prototype for a 'molecular thermometer'.
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Actes de Conférences |
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Chan, A., Clairand, M., Steenkeste, K., Eloy, M., Canette, A., Alousque, F., Ceccia, S., Gaboriaud, F., & Fontaine-Aupart, M. P. (2016). NR – Filler Interactions in aqueous condition by Multi-Modal Fluorescence and Electronic Microscopies. In Communications in Physics (Vol. ISSN 0868).
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Marliere, C. (2016). A direct and at nanometer scale study of electrical charge distribution on membranes of alive cells. In Electro-Activity Of Biological Systems (Vol. 6).
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Monographies |
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Delaire, J., Piard, J., & Méallet-Renault, R. (2016). Photophysique et photochimie: Des fondements aux applications.
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Chapitres de Livres |
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Usami N., Kobayashi K., & Furusawa Y. and Le Sech C. (2016). Hadrontherapy enhanced by combination with heavy atoms : Role of Auger effect in nanoparticles. In Nanobiomaterials in Cancer Therapy. A. Grumezescu Ed. Elsevier Inc (471).
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