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1.
Nanoscale ; 15(43): 17621-17632, 2023 Nov 09.
Article in English | MEDLINE | ID: mdl-37877415

ABSTRACT

Research on graphene-based nanomaterials has experienced exponential growth in the last few decades, driven by their unique properties and their future potential impact on our everyday life. With the increasing production and commercialization of these materials, there is significant interest in understanding their fate in vivo. Herein, we investigated the distribution of 14C-few-layer graphene (14C-FLG) flakes (lat. dim. ∼ 500 nm) in mice over a period of one year. Furthermore, we compared the effects of repeated low-dose and acute high-dose exposure by tracheal administration. The results showed that most of the radioactivity was found in the lungs in both cases, with longer elimination times in the case of acute high-dose administration. In order to gain deeper insights into the distribution pattern, we conducted ex vivo investigations using µ-autoradiography on tissue sections, revealing the heterogeneous distribution of the material following administration. For the first time, µ-autoradiography was used to conduct a comprehensive investigation into the distribution and potential presence of FLG within lung cells isolated from the exposed lungs. The presence of radioactivity in lung cells strongly suggests internalization of the 14C-FLG particles. Overall these results show the long-term accumulation of the material in the lungs over one year, regardless of the administration protocol, and the higher biopersistence of FLG in the case of an acute exposure. These findings highlight the importance of the exposure scenario in the context of intratracheal administration, which is of interest in the evaluation of the potential health risks of graphene-based nanomaterials.


Subject(s)
Graphite , Nanostructures , Animals , Mice , Tissue Distribution , Lung/diagnostic imaging
2.
Nanoscale ; 15(11): 5510-5518, 2023 Mar 16.
Article in English | MEDLINE | ID: mdl-36853236

ABSTRACT

Research on graphene based nanomaterials has flourished in the last decade due their unique properties and emerging socio-economic impact. In the context of their potential exploitation for biomedical applications, there is a growing need for the development of more efficient imaging techniques to track the fate of these materials. Herein we propose the first correlative imaging approach based on the combination of radioimaging and mass spectrometry imaging for the detection of Graphene Oxide (GO) labelled with carbon-14 in mice. In this study, 14C-graphene oxide nanoribbons were produced from the oxidative opening of 14C-carbon nanotubes, and were then intensively sonicated to provide nano-size 14C-GO flakes. After Intravenous administration in mice, 14C-GO distribution was quantified by radioimaging performed on tissue slices. On the same slices, MS-imaging provided a highly resolved distribution map of the nanomaterial based on the detection of specific radical anionic carbon clusters ranging from C2˙- to C9˙- with a base peak at m/z 72 (12C) and 74 (14C) under negative laser desorption ionization mass spectrometry (LDI-MS) conditions. This proof of concept approach synergizes the strength of each technique and could be advantageous in the pre-clinical development of future Graphene-based biomedical applications.


Subject(s)
Graphite , Nanotubes, Carbon , Animals , Mice , Graphite/chemistry , Spectrometry, Mass, Matrix-Assisted Laser Desorption-Ionization/methods , Tissue Distribution , Carbon Radioisotopes
3.
J Am Soc Mass Spectrom ; 31(5): 1025-1036, 2020 May 06.
Article in English | MEDLINE | ID: mdl-32223237

ABSTRACT

Graphene-based nanoparticles are continuously being developed for biomedical applications, and their use raises concerns about their environmental and biological impact. In the literature, some imaging techniques based on fluorescence and radioimaging have been used to explore their fate in vivo. Here, we report on the use of label-free mass spectrometry and mass spectrometry imaging (MSI) for graphene oxide (GO) and reduced graphene oxide (rGO) analyses in rodent tissues. Thereby, we extend previous work by focusing on practical questions to obtain reliable and meaningful images. Specific radical anionic carbon clusters ranging from C2-• to C9-• were observed for both GO and rGO species, with a base peak at m/z 72 under negative laser desorption ionization mass spectrometry (LDI-MS) conditions. Extension to an LDI-MSI method was then performed, thus enabling the efficient detection of GO nanoparticles in lung tissue sections of previously exposed mice. The possibility of quantifying those nanoparticles on tissue sections has also been investigated. Two different ways of building calibration curves (i.e., GO suspensions spotted on tissue sections, or added to lung tissue homogenates) were evaluated and returned similar results, with linear dynamic concentration ranges over at least 2 orders of magnitude. Moreover, intra- and inter-day precision studies have been assessed, with relative standard deviation below 25% for each concentration point of a calibration curve. In conclusion, our study confirms that LDI-MSI is a relevant approach for biodistribution studies of carbon-based nanoparticles, as quantification can be achieved, provided that nanoparticle suspension and manufacturing are carefully controlled.


Subject(s)
Graphite/analysis , Liver/chemistry , Lung/chemistry , Nanoparticles/analysis , Spectrometry, Mass, Matrix-Assisted Laser Desorption-Ionization/methods , Animals , Female , Graphite/administration & dosage , Mice , Mice, Inbred BALB C
4.
Eur J Med Chem ; 94: 386-96, 2015 Apr 13.
Article in English | MEDLINE | ID: mdl-25778994

ABSTRACT

With the aim to develop a suitable radiotracer for the brain imaging of the serotonin 4 receptor subtype (5-HT4R) using single photon emission computed tomography (SPECT), we synthesized and evaluated a library of di- and triazaphenanthridines with lipophilicity values which were in the range expected to favour brain penetration, and which demonstrated specific binding to the target of interest. Adding additional nitrogen atoms to previously described phenanthridine ligands exhibiting a high unspecific binding, we were able to design a radioiodinated compound [(125)I]14. This compound exhibited a binding affinity value of 0.094 nM toward human 5-HT4R and a high selectivity over other serotonin receptor subtypes (5-HTR). In vivo SPECT imaging studies and competition experiments demonstrated that the decreased lipophilicity (in comparison with our previously reported compounds 4 and 5) allowed a more specific labelling of the 5-HT4R brain-containing regions.


Subject(s)
Drug Design , Phenanthridines/pharmacology , Radiopharmaceuticals/pharmacology , Receptors, Serotonin, 5-HT4/metabolism , Tomography, Emission-Computed, Single-Photon , Brain/metabolism , Dose-Response Relationship, Drug , Humans , Iodine Radioisotopes , Ligands , Molecular Structure , Phenanthridines/chemical synthesis , Phenanthridines/chemistry , Radiopharmaceuticals/chemical synthesis , Radiopharmaceuticals/chemistry , Structure-Activity Relationship
5.
Molecules ; 17(12): 14409-17, 2012 Dec 05.
Article in English | MEDLINE | ID: mdl-23519242

ABSTRACT

Following our previous results on an environmentally benign one-pot Sonogashira-cyclization protocol to obtain substituted furopyrimidine nucleosides under aqueous conditions, we investigate herein the Suzuki-Miyaura cross-coupling reactions of aryl and heteroaryl derivatives at the C5 position of unprotected 2'-deoxyuridine in the same media with a common catalyst system avoiding exotic ligands, since palladium acetate and triphenylphosphine afforded the expected products in moderate to good yields.


Subject(s)
Deoxyuridine/analysis , Deoxyuridine/chemical synthesis , Idoxuridine/chemistry , Boronic Acids/chemistry , Catalysis , Ligands , Magnetic Resonance Imaging , Molecular Structure , Organophosphorus Compounds/analysis , Organophosphorus Compounds/chemistry , Palladium/analysis , Palladium/chemistry , Water/analysis
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