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TrAC Trends in Analytical Chemistry 02/2013; · 6.27 Impact Factor
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ABSTRACT: In biological environments, nanomaterials associate with proteins forming a protein corona (PC). The PC may alter the nanomaterial's pharmacokinetics and pharmacodynamics, thereby influencing toxicity. Using a label-free mass spectrometry-based proteomics approach, the composition of the PC is examined for a set of nanotubes (NTs) including unmodified and carboxylated single- (SWCNT) and multi-walled carbon nanotubes (MWCNT), polyvinylpyrrolidone (PVP)-coated MWCNT (MWCNT-PVP), and nanoclay. NTs are incubated for 1 h in simulated cell culture conditions, then washed, resuspended in PBS, and assessed by liquid chromatography-tandem mass spectrometry (LC-MS/MS) for their associated PC. To determine those attributes that influence PC formation, the NTs are extensively characterized. NTs had negative zeta potentials in water (SWCNT-COOH < MWCNT-COOH < unmodified NTs) while carboxylation increases their hydrodynamic sizes. All NTs are also found to associate a common subset of proteins including albumin, titin, and apolipoproteins. SWCNT-COOH and MWCNT-COOH are found to bind the greatest number of proteins (181 and 133 respectively) compared to unmodified NTs (<100), suggesting covalent binding to protein amines. Modified NTs bind a number of unique proteins compared to unmodified NTs, implying hydrogen bonding and electrostatic interactions are involved in PC formation. PVP-coating of MWCNT did not influence PC composition, further reinforcing the possibility of hydrogen bonding and electrostatic interactions. No relationships are found between PC composition and corresponding isoelectric point, hydropathy, or aliphatic index, implying minimal roles of hydrophobic interaction and pi-stacking.
Small 01/2013; · 8.35 Impact Factor
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ABSTRACT: Microwave induced reactions for immobilizing platinum and palladium nanoparticles on multiwall carbon nanotubes are presented. The resulting hybrid materials were used as catalysts for direct methanol, ethanol and formic acid oxidation in acidic as well as alkaline media. The electrodes are formed by simply mixing the hybrids with graphite paste, thus using a relatively small quantity of the precious metal. We report Tafel slopes and apparent activation energies at different potentials and temperatures. Ethanol electro-oxidation with the palladium hybrid showed an activation energy of 7.64 kJmol(-1) which is lower than those observed for other systems. This system is economically attractive because Pd is significantly less expensive than Pt and ethanol is fast evolving as a commercial biofuel.
Electrochimica Acta 11/2012; 83:40-46. · 3.83 Impact Factor
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ABSTRACT: The size dependent colloidal behavior of aqueous dispersions of carboxylated multiwall carbon nanotubes (c-MWCNTs) is presented. The presence of carboxylic groups provided electrostatic stabilization in water, where the size affected agglomeration. While aspect ratio did not show any definite correlation, the hydrophobicity indices (HI), zeta potential and aggregation kinetics showed dependence on the length of the c-MWCNTs where the shorter c-MWCNTs showed significantly lower HI values, smaller particle aggregates, higher zeta potential values and higher critical coagulation concentrations (ccc) in the presence of electrolytes. Although the diameter of the short c-MWCNTs did not appear to influence their aggregation behavior, the longer c-MWCNTs showed a dependence on diameter where stability decreased with increasing CNT diameter.
Journal of Environmental Monitoring 09/2012; 14(10):2772-9. · 1.99 Impact Factor
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ABSTRACT: Size dependent colloidal behavior of aqueous dispersions of carboxylated multiwall carbon nanotubes (c-MWCNTs) is presented. The presence of carboxylic groups provided electrostatic stabilization in water, where the size affected agglomeration. While aspect ratio did not show any definite correlation, the hydrophobicity indices (HI), Zeta potential and aggregation kinetics showed dependence on the length of the c-MWCNTs where the shorter c-MWCNTs showed significantly lower HI values, smaller particle aggregates, higher zeta potential values and higher critical coagulation concentrations (ccc) in the presence of electrolytes. Although the diameter of the short c-MWCNTs did not appear to influence their aggregation behavior, the longer c-MWCNTs showed a dependence on diameter where stability decreased with increasing CNT diameter.
Journal of Environmental Monitoring. 08/2012;
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ABSTRACT: We demonstrate for the first time that carbon nanotubes (CNTs) can be readily immobilized on the surface of a solid polymeric membrane which can lead to enhanced enrichment factor and extraction efficiency. The effectiveness of the CNT mediated process is demonstrated by micro-scale membrane extraction via direct solvent enrichment of polar and nonpolar organics. The enrichment factor measured as the ratio of concentrations in the acceptor to the donor phases was as high as 282 and the enhancement over the unmodified membrane was as much as 92%. In addition, the solvent retention in the carbon nanotube immobilized membrane (CNIM) increased by as much as 29%. Overall, the CNT incorporation provided enhanced solute transport and thus led to overall performance enhancement.
The Analyst 08/2012; 137(19):4464-8. · 4.23 Impact Factor
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ABSTRACT: Single-wall carbon nanotubes (SWNTs) provide a reactive environment in presence of microwave radiation because they absorb
the energy that leads to fast, direct heating. This makes composite formation in a microwave reactor highly feasible where
the SWNTs serve as the nuclei for polymerization. In this article, we demonstrate rapid, insitu synthesis of poly(methyl
methacrylate) (PMMA) and polyvinylpyrrolidone (PVP) nanocomposites using their respective monomers. The key to their success
was the use of the highly dispersible SWNTs, which had strong interactions with the monomer and the polymer. Rapid synthesis
within a few minutes was possible, which led to remarkable nano-scale dispersion of nanotubes in polymer matrix by encapsulation
of the already dispersed SWNTs before the latter could agglomerate. The molecular weight and polydispersity of the polymers
remained unchanged in the presence of the SWNTs. The addition of 0.5wt% SWNT to PMMA enhanced its thermal stability (as measured
by the initial degradation temperature) by 37°C and the hardness by around 50%. On the other hand, with the addition of up
to 4wt% SWNT, the PVP showed no enhancement in thermal stability but its hardness increased by 250–300%. Finally, this technique
is practical because it reduces time, cost, and energy requirements.
Journal of Materials Science 04/2012; 44(5):1245-1250. · 2.02 Impact Factor
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ABSTRACT: The adsorptive removal of arsenic from water using a multiwall carbon nanotube-zirconia nanohybrid (MWCNT-ZrO(2)) is presented. The MWCNT-ZrO(2) with 4.85% zirconia was effective in meeting the drinking water standard levels of 10 μg L(-1). The absorption capacity of the composite were 2000 μg g(-1) and 5000 μg g(-1) for As(III) and As(V) respectively, which were significantly higher than those reported previously for iron oxide coated MWCNTs. The adsorption of As(V) on MWCNT-ZrO(2) was faster than that of As(III), and a pseudo-second order rate equation effectively described the uptake kinetics. The adsorption isotherms for As(III) and As(V) fitted both the Langmuir and Freundlich models. A major advantage of the MWCNT-ZrO(2) was that the adsorption capacity was not a function of pH.
Journal of Colloid and Interface Science 02/2012; 375(1):154-9. · 3.07 Impact Factor
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ABSTRACT: The anti-solvent synthesis in presence of cyclodextrins (CDs) of the drug Griseofulvin (GF) is presented. This was followed by immobilization into cellulosic polymer films suitable for drug delivery. The results show that 72% of the GF precipitated in presence of CD, while the rest led to the formation of a water soluble GF/CD complex. The cyclodextrins were effective in inhibiting particle growth and stabilizing the drug suspensions. Among the CDs tested here, hydroxypropyl-β-cyclodextrin (HPBCD) was found to be most effective in reducing the particle size. The release profiles from the cyclodextrin stabilized GF particles showed improvement in release rate, which indicated effective drug/cyclodextrin interactions.
Colloids and surfaces. B, Biointerfaces 12/2011; 92:213-22. · 2.60 Impact Factor
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ABSTRACT: The possibility of antisolvent precipitation of hydrophobic, organic soluble functionalized carbon nanotubes (f-CNTs), where water acts as an antisolvent is presented. Octadecylamine functionalized multiwall carbon nanotubes (MWCNT-ODA) was used as the model compound and was found to form highly stable dispersions in different water/solvent systems, and the particle sizes ranged from 170 to 400 nm. Colloidal behavior was studied using dynamic light scattering and particle aggregation was found to increase with the addition of electrolytes, with tetrahydrofuran (THF) and ethanol showing the maximum effect. The aggregation behavior of the antisolvent precipitated system did not follow the conventional Derjaguin-Landau-Verwey-Overbeek (DLVO) theory, which was different from what has been reported previously for hydrophilic, water soluble f-CNTs. Based on this study, it is evident that hydrophobic f-CNTs are potential water pollutants.
Journal of Colloid and Interface Science 11/2011; 368(1):115-20. · 3.07 Impact Factor
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ABSTRACT: In this paper, we report the implementation of polar and nonpolar functionalized multiwalled carbon nanotubes (MWCNTs) as sorbent in μ-SPE integrated into the needle of a syringe. Excellent preconcentration of diverse pharmaceutical analytes was possible without the need for specific pH adjustments using just 300 μg of functionalized nanotubes. Enrichment factors were as high as 6.4, extraction efficiencies were as high as 25.6%, and detection limits as low as 0.08 ng/ml were obtained. The sorption on nanotubes followed Freundlich isotherms, and it was seen that polar analytes adsorbed more strongly on carboxylated MWCNTs, while amphoteric, relatively less polar and basic analytes had greater affinity for MWCNT and those with octadecylamine functionalization.
Analytical and Bioanalytical Chemistry 11/2011; 402(3):1029-39. · 3.78 Impact Factor
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Xiang Wang,
Tian Xia,
Susana Addo Ntim,
Zhaoxia Ji,
Sijie Lin,
Huan Meng,
Choong-Heui Chung,
Saji George,
Haiyuan Zhang,
Meiying Wang,
Ning Li,
Yang Yang,
Vincent Castranova, Somenath Mitra,
James C Bonner,
André E Nel
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ABSTRACT: We developed a dispersal method for multiwalled carbon nanotubes (MWCNTs) that allows quantitative assessment of dispersion on profibrogenic responses in tissue culture cells and in mouse lung. We demonstrate that the dispersal of as-prepared (AP), purified (PD), and carboxylated (COOH) MWCNTs by bovine serum albumin (BSA) and dipalmitoylphosphatidylcholine (DPPC) influences TGF-β1, PDGF-AA, and IL-1β production in vitro and in vivo. These biomarkers were chosen based on their synergy in promoting fibrogenesis and cellular communication in the epithelial-mesenchymal cell trophic unit in the lung. The effect of dispersal was most noticeable in AP- and PD-MWCNTs, which are more hydrophobic and unstable in aqueous buffers than hydrophilic COOH-MWCNTs. Well-dispersed AP- and PD-MWCNTs were readily taken up by BEAS-2B, THP-1 cells, and alveolar macrophages (AM) and induced more prominent TGF-β1 and IL-1β production in vitro and TGF-β1, IL-1β, and PDGF-AA production in vivo than nondispersed tubes. Moreover, there was good agreement between the profibrogenic responses in vitro and in vivo as well as the ability of dispersed tubes to generate granulomatous inflammation and fibrosis in airways. Tube dispersal also elicited more robust IL-1β production in THP-1 cells. While COOH-MWCNTs were poorly taken up in BEAS-2B and induced little TGF-β1 production, they were bioprocessed by AM and induced less prominent collagen deposition at sites of nongranulomatous inflammation in the alveolar region. Taken together, these results indicate that the dispersal state of MWCNTs affects profibrogenic cellular responses that correlate with the extent of pulmonary fibrosis and are of potential use to predict pulmonary toxicity.
ACS Nano 11/2011; 5(12):9772-87. · 10.77 Impact Factor
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ABSTRACT: The anti-solvent synthesis of micron-scale particles, their stabilization, and subsequent self-assembly into polymer films suitable for drug delivery is presented. The colloidal particles were stabilized using low molecular weight hydroxypropyl methylcellulose (HPMC), while drug encapsulation was carried out with high molecular weight HPMC and polyvinylpyrrolidone (PVP). Griseofulvin (GF) was used as the model drug compound, and the polymer films were evaluated in terms of their surface morphology, mechanical properties and in vitro drug release. In general, the release rates were best described by first-order and Hixson-Crowell kinetic models, and in a typical film containing 57% HPMC, 100% of GF was released within 50 min.
Colloids and surfaces. B, Biointerfaces 08/2011; 86(1):181-8. · 2.60 Impact Factor
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ABSTRACT: Carbon nanotube enhanced membrane distillation (MD) is presented as a novel, online analytical preconcentration method for removing polar solvents thereby concentrating the analytes, making this technique an alternate to conventional thermal evaporation. In a carbon nanotube immobilized membrane (CNIM), the CNTs serve as sorbent sites and provide additional pathways for enhanced solvent vapor transport, thus enhancing preconcentration. Enrichment using CNIM doubled compared to membranes without CNTs, while the methanol flux and mass transfer coefficients increased by 61% and 519% respectively. The carbon nanotube enhanced MD process showed excellent precision (RSD of 3-5%), linearity, and the detection limits were in the range of 0.001 to 0.009 mg L(-1) by HPLC analysis.
The Analyst 06/2011; 136(12):2643-8. · 4.23 Impact Factor
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ABSTRACT: This study presents the removal of trace level arsenic to meet drinking water standards using an iron oxide-multi-walled carbon nanotube (Fe-MWCNT) hybrid as a sorbent. The synthesis was facilitated by the high degree of nanotube functionalization using a microwave assisted process, and a controlled assembly of iron oxide was possible where the MWCNT served as an effective support for the oxide. In the final product, 11 % of the carbon atoms were attached to Fe. The Fe-MWCNT was effective in arsenic removal to below the drinking water standard levels of 10 µg L(-1). The absorption capacity of the composite was 1723 µg g(-1) and 189 µg g(-1) for As(III) and As(V) respectively. The adsorption of As(V) on Fe-MWCNT was faster than that of As(III). The pseudo-second order rate equation was found to effectively describe the kinetics of arsenic adsorption. The adsorption isotherms for As(III) and As(V) fitted both the Langmuir and Freundlich models.
Journal of Chemical & Engineering Data 05/2011; 56(5):2077-2083. · 1.69 Impact Factor
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ABSTRACT: This study presents the synthesis of zirconia/multi-walled carbon nanotube (ZrO2/MWCNTs) hybrid as a novel sorbent for water defluoridation. The synthesis was facilitated by the high degree of functionalization of MWCNTs using a microwave assisted process. In the final product, nearly 3% of the carbon atoms were attached to ZrO2. The ZrO2/MWCNTs were effective in fluoride removal and mechanistic aspects of the process are presented. The research findings highlight the potential application for the use of MWCNT hybrids in environmental remediation.
Journal of Nanoscience and Nanotechnology 04/2011; 11(4):3552-9. · 1.56 Impact Factor
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Journal of Membrane Science 03/2011; · 3.85 Impact Factor
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ABSTRACT: The colloidal behavior of aqueous dispersions of functionalized multiwall carbon nanotubes (F-CNTS) formed via carboxylation and polymer wrapping with polyvinyl pyrrolidone (PVP) is presented. The presence of polymer on the nanotube surface provided steric stabilization, and the aggregation behavior of the colloidal system was quite different from its covalently functionalized analog. Based on hydrophobicity index, particle size distribution, zeta potential as well as the aggregation kinetics studied using time-resolved dynamic light scattering, the PVP wrapped CNT was somewhat less prone to agglomeration. However, its long-term stability was lower, and this was attributed to the partial unwrapping of the polyvinyl pyrrolidone layer on the CNT surface.
Journal of Colloid and Interface Science 03/2011; 355(2):383-8. · 3.07 Impact Factor
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ABSTRACT: It is currently of great interest to the pharmaceutical industry to control the size and agglomeration of nano- and micro-particles for the enhancement of drug delivery. Typically, surfactants and polymers are used as additives to interact with and stabilize the growing crystal surface, thus controlling size and agglomeration; however, selection is traditionally done empirically or using heuristics. The objective of this study was to use molecular dynamic simulations to investigate and predict additive interactions, and thus, evaluate the stabilization potential of individual and multiple additives on the surface of the model drug fenofibrate. Non-ionic surfactant Tween 80, anionic surfactant sodium dodecyl sulfate (SDS), and polymers hydroxypropyl methylcellulose (HPMC) and Pullulan were evaluated individually on three distinct crystal surfaces [(001), (010), (100)], as well as in surfactant-polymer combinations. HPMC was determined to have the strongest interaction with the surfaces of the fenofibrate crystal, and therefore, was predicted to be the most effective individual additive. A mixture of HPMC with SDS was determined to be the most effective mixture of additives, and more effective than HPMC alone, indicating a synergistic effect. The predictions of mixed additives indicated a relative order of effectiveness as follows: HPMC-SDS>HPMC-Tween 80>Pullulan-Tween 80>Pullulan-SDS. The simulations were subsequently validated by an anti-solvent crystallization of fenofibrate where it was found that HPMC individually, and a mixture of HPMC-SDS, produced the smallest and most stable crystals, as measured by laser diffraction; this, in combination with measurements of the crystal growth rate in the presence and absence of additives confirmed the results of the simulations.
European journal of pharmaceutical sciences: official journal of the European Federation for Pharmaceutical Sciences 02/2011; 42(5):452-61. · 2.61 Impact Factor
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ABSTRACT: Membrane distillation (MD) is presented for the first time as a real-time, online concentration technique, where the aqueous matrix is removed from the sample to enhance analyte enrichment. Therefore, MD is a universal method for a wide range of compounds and is unlike conventional membrane extractions that rely on the permeation of the solute into an extractant phase. The MD process showed excellent precision with relative standard deviation between 3% and 5%, linear calibration, and the detection limits for pharmaceutical compounds in the range of 0.01 to 20 mg L(-1) by HPLC-UV analysis. The temperature and flow rate of the feed solution were found to be important variables.
Analytical and Bioanalytical Chemistry 02/2011; 400(2):571-5. · 3.78 Impact Factor
