Hydration and Dispersion of C<sub>60</sub> in Aqueous Systems: The Nature of Water−Fullerene Interactions

Labille, Jérôme; Armand, Michel; Ziarelli, Fabio; Rose, Jérôme; Brant, Jonathan A.; Villièras, Frédéric; Pelletier, Manuel; Borschneck, Daniel; Wiesner, Mark R.; Bottero, Jean‐Yves

doi:10.1021/la9022807

Cited by 106 publications

(113 citation statements)

References 29 publications

(35 reference statements)

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“…The hydroxylation of the fullerene cage found in the present work for C 60 FAS prepared by method 2 is in agreement with the same experimental evidence reported in ref 18 by FTIR for C 60 FAS prepared by method 1. It strongly suggests that the primary mechanism of C 60 fullerene solubilization in water is the attachment of the OH groups to C 60 fullerene carbons, which explains why the lone C 60 molecules and their clusters exist at equilibrium in solution for quite a long time (see above), a feature that is independent of the method of C 60 FAS preparation.…”

Section: ■ Results and Discussionsupporting

confidence: 93%

“…17 The covalent attachment of the OH groups does not exclude the possibility of electron transfer from water molecules to C 60 fullerene, enabling us to explain the negative charge on fullerene particles. 17,18,28 However, the previous model of stabilization of hydrated C 60 fullerene by water molecules joined together by an H-bonding network 17,23 needs to be corrected in view of the available results of molecular dynamics simulations of hydrated C 60 fullerenes 29,30 reporting the weakening and breakage of the H bonds between water molecules in the immediate vicinity of the C 60 fullerene surface as a result of the overbalancing effect of C 60 fullerene−water with respect to the water−water interaction.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

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On the Origin of C₆₀ Fullerene Solubility in Aqueous Solution

et al. 2014

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In this work, we report that the surface hydroxylation of C 60 molecules is the most likely mechanism for pristine C 60 fullerenes/C 60 fullerene aggregate stabilization in water, being independent of the method of C 60 fullerene aqueous solution preparation. ■ INTRODUCTIONNanocarbon materials are used in a wide variety of biomedical applications, including biosensorics, targeted drug delivery, chemotherapy, cellular imaging, and diagnostics. 1 For example, the pristine C 60 fullerenes as a unique class of carbon allotropes are able to penetrate the cell membrane, 2,3 to exhibit antioxidant properties, 4,5 and, being nontoxic (at least at low concentration), 6 to exert specific health effects (e.g., antibacterial, 7 antitumor, 8 and drug carrier 9 ).Biomedical applications require a dispersal of C 60 fullerene in a solvent, with aqueous dispersions being preferred because of biocompatibility, safety, or environmental concerns. Although pristine C 60 fullerenes have extremely low water solubility, they can form stable colloid solutions containing individual C 60 fullerenes as well as C 60 fullerene aggregates (clusters) in water when subjected to extended mixing, sonication, or solvent exchange 10−16 (to be further referred to as a C 60 fullerene aqueous colloid solution (C 60 FAS)). However, the origin of stabilization of such particles in water still remains poorly investigated.At least two approaches have been suggested in order to explain the stability of fullerene particles in water solutions. One of them 17 postulates the formation of a water shell around C 60 molecules stabilized simultaneously by the H-bonding network between the water molecules and charge transfer from water to the C 60 fullerene. Another one 18 suggests that the sonication process induces the covalent attachment of water hydroxyls to C 60 fullerene carbons, resulting in the formation of alcohol moieties that enable C 60 fullerene dissolution. The problem here is that the properties of C 60 FAS (including biological properties) as well as the mechanism of water solubility may depend on the method of preparation of C 60 fullerene aqueous solution. 13,16,17 Indeed, these two approaches differ by the underlying method of C 60 FAS preparation although the sonication step is presented in both methods. The question therefore arises as to whether the mechanism of solubility of C 60 fullerene in water depends on the method of C 60 FAS preparation. This question has been investigated in this article. ■ EXPERIMENTAL SECTIONSample Preparation. For the preparation of C 60 FAS, we used a saturated solution of pure C 60 fullerene (purity >99.99%) in toluene with a C 60 molecule concentration corresponding to maximum solubility near 2.9 mg/mL and the same amount of distilled water in an open beaker. The two phases that formed were treated in an ultrasonic bath. The procedure was continued until the toluene had completely evaporated and the water phase became yellow. Filtration of the aqueous solution allowed us to separate the product from un...

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Section: ■ Results and Discussionsupporting

confidence: 93%

Section: ■ Results and Discussionmentioning

confidence: 99%

On the Origin of C₆₀ Fullerene Solubility in Aqueous Solution

et al. 2014

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“…The effective permeability decreases upon increasing the volume fraction of impermeable nanoparticles and is believed to be the result of the reduction in membrane solubility due to the decrease in polymer content, and of diffusivity reduction due to the increase of the penetrant diffusion pathway length (Cong et al, 2007). However, in general, the addition of fullerene to polymers decreases permeability more than the loss (14%) predicted by Maxwell's model (Saga et al, 2008;Ong et al, 2006;Polotskaya et al, 2006;Labille et al, 2009). Additionally, non-Maxwellian behavior has been observed in numerous other polymer-inorganic nanocomposite membranes.…”

Section: Modeling Gas Transport Properties In Nanocomposite Membranesmentioning

confidence: 99%

Organic-inorganic hybrid membranes in separation processes: a 10-year review

Souza

Quadri

2013

Braz. J. Chem. Eng.

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-In relation to some inorganic membranes, polymeric membranes have relatively low separation performance. However, the processing flexibility and low cost of polymers still make them highly attractive for many industrial separation applications. Polymer-inorganic hybrid membranes constitute an emerging research field and have been recently developed to improve the separation properties of polymer membranes because they possess properties of both organic and inorganic membranes such as good hydrophilicity, selectivity, permeability, mechanical strength, and thermal and chemical stability. The structures and processing of polymer-inorganic nanocomposite hybrid membranes, as well as their use in the fields of ultrafiltration, nanofiltration, pervaporation, gas separation and separation mechanism are reviewed.

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“…Some possible methods include the stirring of C 60 crystals in water for a prolonged period of time (from 2 weeks to 5 months) [134][135][136][137][138] and ultrasonication of C 60 crystals in water. [139,140] Colloidal stability The unusual colloidal stability of the supposedly hydrophobic C 60 nanoparticles has been highlighted in numerous studies. [132,[141][142][143] Specifically, C 60 nanoparticles are found to be extremely stable to aggregation under low ionic-strength conditions regardless of the synthesis method used, and even in the absence of surfactants or stabilisers, they have been reported to remain colloidally stable for months.…”

Section: Preparation Of C 60 Colloidsmentioning

confidence: 99%

Assessing the colloidal properties of engineered nanoparticles in water: case studies from fullerene C60 nanoparticles and carbon nanotubes

Chen¹,

Smith²,

Ball³

et al. 2010

Environ. Chem.

134

114

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Environmental context. The fate and bioavailability of engineered nanoparticles in natural aquatic systems are strongly influenced by their ability to remain dispersed in water. Consequently, understanding the colloidal properties of engineered nanoparticles through rigorous characterisation of physicochemical properties and measurements of particle stability will allow for a more accurate prediction of their environmental, health, and safety effects in aquatic systems.This review highlights some important techniques suitable for the assessment of the colloidal properties of engineered nanoparticles and discusses some recent findings obtained by using these techniques on two popular carbon-based nanoparticles, fullerene C 60 and multi-walled carbon nanotubes.Abstract. The colloidal properties of engineered nanoparticles directly affect their use in a wide variety of applications and also control their environmental fate and mobility. The colloidal stability of engineered nanoparticles depends on their physicochemical properties within the given aqueous medium and is ultimately reflected in the particles' aggregation and deposition behaviour. This review presents some of the key experimental methods that are currently used to probe colloidal properties and quantify engineered nanoparticle stability in water. Case studies from fullerene C 60 nanoparticles and multi-walled carbon nanotubes illustrate how the characterisation and measurement methods are used to understand and predict nanoparticle fate in aquatic systems. Consideration of the comparisons between these two classes of carbonbased nanoparticles provides useful insights into some major current knowledge gaps while also revealing clues about needed future developments. Key issues to be resolved relate to the nature of near-range surface forces and the origins of surface charge, particularly for the reportedly unmodified or 'pure' carbon-based nanoparticles.

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Hydration and Dispersion of C₆₀ in Aqueous Systems: The Nature of Water−Fullerene Interactions

Cited by 106 publications

References 29 publications

On the Origin of C₆₀ Fullerene Solubility in Aqueous Solution

On the Origin of C₆₀ Fullerene Solubility in Aqueous Solution

Organic-inorganic hybrid membranes in separation processes: a 10-year review

Assessing the colloidal properties of engineered nanoparticles in water: case studies from fullerene C60 nanoparticles and carbon nanotubes

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Hydration and Dispersion of C60 in Aqueous Systems: The Nature of Water−Fullerene Interactions

Cited by 106 publications

References 29 publications

On the Origin of C60 Fullerene Solubility in Aqueous Solution

On the Origin of C60 Fullerene Solubility in Aqueous Solution

Organic-inorganic hybrid membranes in separation processes: a 10-year review

Assessing the colloidal properties of engineered nanoparticles in water: case studies from fullerene C60 nanoparticles and carbon nanotubes

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Product

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Hydration and Dispersion of C₆₀ in Aqueous Systems: The Nature of Water−Fullerene Interactions

On the Origin of C₆₀ Fullerene Solubility in Aqueous Solution

On the Origin of C₆₀ Fullerene Solubility in Aqueous Solution