High Relaxivity Trimetallic Nitride (Gd<sub>3</sub>N) Metallofullerene MRI Contrast Agents with Optimized Functionality

Zhang, Jianfei; Fatouros, Panos P.; Shu, Chunying; Reid, Jonathan E.; Owens, L.; Cai, Ting; Gibson, Harry W.; Long, Gary L.; Corwin, Frank; Chen, Zhijian; Dorn, Harry C.

doi:10.1021/bc900375n

Cited by 130 publications

(135 citation statements)

References 28 publications

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“…stabilizing the metal ion using a chelating agent (for example DTPA or DOTA) but recently several other strategies have been proposed. Among these, metallofullerenes where the Gd ions are encapsulated in a fullerene cage (Toth et al 2005;Shu et al 2009;Zhang et al 2010a;Bolskar et al 2003), metal-organic frameworks (MOFs) (Rowe et al 2009b;Rieter et al 2006;Rowe et al 2009a) and nanoscale coordination polymers (NCP) (Zhang et al 2010b) can be mentioned. The synthesis of the latter compounds, however, is typically quite complicated normally involving several steps.…”

Section: Introductionmentioning

confidence: 99%

A simple polyol-free synthesis route to Gd2O3 nanoparticles for MRI applications: an experimental and theoretical study

et al. 2012

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In all kinds of gadolinium based contrast agents, the presence of free gadolinium ions have to be avoided due to the cytotoxicity. The conventional way of producing a gadolinium based contrast agent is to form a chelate, i.e. stabilizing the metal ion using a chelating agent (for example DTPA or DOTA) but recently nanoparticles is an initial step towards biocompatible and directed nanoparticles.The main focus is on a material that in the nearby future will be the core of an The experimental results are supported by theoretical modeling studies.Theoretical IR spectra of three different Gd acetate complexes are presented as well as calculated NEXAFS spectra of one of the Gd acetate complexes and an isolated acetate group. These calculations were performed to elucidate the molecular capping of the synthesized particles. 5 EXPERIMENTAL DETAILS ChemicalsAll chemicals were used as received. Gadolinium(III) acetate hydrate (SigmaAldrich, 99.9 %), tetramethylammonium hydroxide (Sigma-Aldrich, >97 % ), ethyl acetate (Fisher Scientific, 99.99 %), dimethyl sulfoxide (Merck, 99.9 %), ammonium acetate (Merck, >96%), ethanol (Kemetyl, 99.5 %). For preparation of water based solutions, Milli-Q water (ρ > 18.2 MΩ) was used. A commercial gadolinium oxide nanopowder (Aldrich, < 100 nm, 99.8 %) was used as a reference. Preparation of Gd 2 O 3 nanoparticlesThe preparation of Gd 2 O 3 nanoparticles was based on a method previously used for producing nanocrystalline ZnO (Schwartz et al. 2003). As Zn 2+ is divalent and Ethyl acetate was added and the mixture was centrifuge washed (3500 rpm) at least three times with ethyl acetate before it was diluted in deionized water. A total amount of 0.28 g ammonium acetate was added to one whole batch to increase the water solubility. Powder samples were air dried. The yield of the sample is dependent on the washing procedure. The gadolinium content after three times of centrifuge washing with ethyl acetate is roughly 60-65 % of the initial amount added in the synthesis.6 Instrumentation X-ray diffraction XRD measurements were carried out with a Philips XRD powder diffractometer using Cu Kα radiation (λ = 1.5418 Å, 40kV, 40 mA). The 2θ step-size was 0.025° and the time per step 4 s. Air dried powder samples were used in the preparation.High-resolution transmission electron microscopy TEM measurements were performed on a FEI Tecnai G 2 electron microscope operated at 200 kV. Sample preparation was done by letting 1-2 drops of Gd 2 O 3 in water dry on an amorphous carbon-covered copper grid.Dynamic light scattering DLS measurements were carried out on an ALV/DLS/SLS-5022F system from ALV-GmbH, Langen Germany, using a HeNe laser at 632.8 nm with 22 mW output power. Prior to the measurements, the samples were temperature stabilized in a thermostat bath at 22.1 °C for at least 10 minutes. The scattering angle was 90°. 15 Gd 2 O 3 samples dispersed in MilliQ water were studied in DLS, and the long term stability of the suspensions were studied by repeated measurements during a period of 6 weeks.ζ Pot...

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Section: Introductionmentioning

confidence: 99%

A simple polyol-free synthesis route to Gd2O3 nanoparticles for MRI applications: an experimental and theoretical study

et al. 2012

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“…In order to determine the labeling efficiency, the total activity of the 3 fractions containing the Fraction #8 contained both the highest 124 I activity and f-Gd 3 N@C 80 concentration and thus was further subjected to HPLC analysis with UV/radioactive detection in order to determine the radiochemical purity. As the f-Gd 3 N@C 80 nanoplatform has been extensively characterized in the literature [34][35][36][37]41,43,44], it was possible to obtain the radiochemical purity by HPLC separation. This was due to the high purity of the f-Gd 3 N@C 80 starting material which would only yield three possible products following the iodination reaction, namely f-Gd 3 N@C 80 , 124 I-f-Gd 3 N@C 80 , and free 124 I.…”

Section: Resultsmentioning

confidence: 99%

“…Altering the endohedral metal is the basic method for endowing additional imaging properties to the fullerene. Examples of this include encapsulation of Gd or Gd 3 N for superior MRI contrast [34,35], Lu 3 N for x-ray contrast [36], and 177 Lu for SPECT detection [37]. External ligands have also been added to empty C 60 cages to provide x-ray contrast [38,39] and radiolabeling [40].…”

Section: Introductionmentioning

confidence: 99%

A Dual PET/MR Imaging Nanoprobe: 124I Labeled Gd3N@C80

et al. 2012

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Abstract:The current report describes the development of a dual modality tomographic agent for both positron emission tomography and magnetic resonance imaging (PET/MRI). The dual-modality agent in this study was based on a 124 I (PET) radiolabeled tri-gadolinium endohedral metallofullerene Gd 3 N@C 80 (MRI) nanoprobe platform. The outer surface of the fullerene cage of the Gd 3 N@C 80 metallofullerenes was surface functionalized with carboxyl and hydroxyl groups (f-Gd 3 N@C 80 ) using previously developed procedures and subsequently iodinated with I-f-Gd 3 N@C 80 , which could ultimately be used for simultaneous PET/MR imaging.

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“…For example, the system Gd 3 N@C 80 [DiPEG(OH) x ] with two PEG units at the exohedral carbon atom shows the highest relaxivity among the EMF derivatives used as MRI contrast agents. 343 Endometallofullerenes are suitable for the design of not only contrast agents for MRI, but also other methods of investigation. For example, an atherosclerotic-targeting contrast agent can be prepared on the basis of Gd 3 N@C 80 .…”

Section: Iii3 Biomedical Applicationsmentioning

confidence: 99%

Fullerene derivatives as nano-additives in polymer composites

Penkova¹,

Acquah²,

Piotrovskiy³

et al. 2017

Russ. Chem. Rev.

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High Relaxivity Trimetallic Nitride (Gd₃N) Metallofullerene MRI Contrast Agents with Optimized Functionality

Abstract: The water soluble poly(ethylene glycol) (PEG) functionalized and hydroxylated endohedral trimetallic nitride metallofullerene derivatives, Gd 3 N@C 80 [DiPEG(OH)

Cited by 130 publications

References 28 publications

A simple polyol-free synthesis route to Gd2O3 nanoparticles for MRI applications: an experimental and theoretical study

A simple polyol-free synthesis route to Gd2O3 nanoparticles for MRI applications: an experimental and theoretical study

A Dual PET/MR Imaging Nanoprobe: 124I Labeled Gd3N@C80

Fullerene derivatives as nano-additives in polymer composites

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High Relaxivity Trimetallic Nitride (Gd3N) Metallofullerene MRI Contrast Agents with Optimized Functionality

Abstract: The water soluble poly(ethylene glycol) (PEG) functionalized and hydroxylated endohedral trimetallic nitride metallofullerene derivatives, Gd 3 N@C 80 [DiPEG(OH)

Cited by 130 publications

References 28 publications

A simple polyol-free synthesis route to Gd2O3 nanoparticles for MRI applications: an experimental and theoretical study

A simple polyol-free synthesis route to Gd2O3 nanoparticles for MRI applications: an experimental and theoretical study

A Dual PET/MR Imaging Nanoprobe: 124I Labeled Gd3N@C80

Fullerene derivatives as nano-additives in polymer composites

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High Relaxivity Trimetallic Nitride (Gd₃N) Metallofullerene MRI Contrast Agents with Optimized Functionality