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We investigate several ion transport behaviors in sub-20 nm nanofluidic channels consisting of heterogeneous oxide materials. By utilizing distinct isoelectric points of SiO2 and Al2O3 surfaces and photolithography to define the charge distribution, nanofluidic channels containing positively and negatively charged surfaces are created to form an abrupt junction. This method provides much more robust surface charges than previous approaches by surface chemical treatment. The fabricated nanofluidic diodes exhibit high rectification of ion current and achieve record-high rectification factors (ratio of forward current to reverse current) of over 300. The current-voltage property of the device follows the theoretical model quantitatively, except that at low ion concentrations the forward current degrades and the reverse current is greater than theoretical prediction, which can be attributed to access resistance and breakdown of water molecules. The breakdown effect characterized by a negative conductance followed by a rapid increase of current is observed in a double junction diode. The occurrence of the breakdown is found to be enhanced by the abruptness of the junction between the heterogeneous nanochannels. Finally, we demonstrate ionic switching in a three-terminal nanofluidic triode in which the ionic flow can be electrically regulated between different channel branches. The study provides insight into the ion transport behavior in nanofluidic devices containing heterogeneous surfaces.
ACS Nano 2009 Mar 24
PMID:Ionic current rectification, breakdown, and switching in heterogeneous oxide nanofluidic devices. 1922 10

Ttrioctylphosphine oxide (TOPO) stabilized CdSe/ZnS quantum dots (QD) were modified with 6-ferrocenyl-1-hexanethiol (FcHT) or 11-ferrocenyl-1-undecanethiol (FcUT) via ligand exchange. The presence of ferrocenyl thiol ligands on the surface of the QDs was proven by diffusion ordered NMR spectroscopy. Upon replacement of the initial TOPO ligand with ferrocene derivatives the emission of the QDs decreased. Phase transfer of ferrocene-modified QDs from organic solvents into water was achieved by complexation reactions with beta-cyclodextrin (beta-CD). The QDs coated with ferrocene thiols are soluble in nonpolar solvents and are transferred into the aqueous phase upon formation of host-guest complexes between the ferrocene units and the cavity of beta-CD. The reversibility of the phase transfer was probed by the addition of naphthalene and adamantane derivatives to the aqueous phase containing QD-[Fc-CD] adduct.
ACS Nano 2009 Mar 24
PMID:Reversible phase transfer of (CdSe/ZnS) quantum dots between organic and aqueous solutions. 1923 90

Periodic density functional calculations are carried out to investigate the structure and the stability of hydrated/hydroxylated TiO(2) layered compounds, nanosheets, and nanotubes. Due to a very efficient interlayer hydrogen bonding, the ABA-stacked "step 3" H(2)Ti(3)O(7) compound is found to be the most stable bulk phase, in agreement with the experiment. For single sheets in a water-rich environment other forms are instead favored, all close in energy, namely, "step 2" titanates, hydroxylized-anatase-like layers, and lepidocrocite-TiO(2). Finally, it is shown that a lepidocrocite-TiO(2) sheet, when hydroxylated only on one side, spontaneously forms a scroll-like nanotube. The nanotube diameter estimated from our models perfectly matches the approximately 3 nm value observed for the internal diameters of Na-free titania nanotubes.
ACS Nano 2009 Feb 24
PMID:First principles study of hydrated/hydroxylated TiO2 nanolayers: from isolated sheets to stacks and tubes. 1923 66

Synthesis of ultrasmall water-soluble fluorescent gold nanoclusters is reported. The clusters have a decent quantum yield, high colloidal stability, and can be readily conjugated with biological molecules. Specific staining of cells and nonspecific uptake by living cells is demonstrated.
ACS Nano 2009 Feb 24
PMID:Synthesis, characterization, and bioconjugation of fluorescent gold nanoclusters toward biological labeling applications. 1923 77

Many types of metal and semiconductor nanoparticles (NPs) are created via colloidal synthetic methods, which renders the materials hydrophobic. Such NPs are dispersed in water through surface organic cap exchange or by amphiphilic polymer encapsulation; often, water solubility is achieved via the presence of carboxylic acid functionalities on the solubilizing agents. While this renders the material water-soluble, subsequent functionalization of the systems can be very difficult. The most obvious method to derivatize carboxylic acid coated NPs is to conjugate chemical and biological moieties containing amine functionality to the NP surface using the water-soluble activator 1-ethyl-3-(3-dimethylaminopropyl) carbodiimide hydrochloride (EDC). However, the excess use of this reagent appears to cause complete and permanent precipitation of the NPs. We report here our method on the chemical and biological functionalization of a variety of semiconductor nanoparticle systems using novel carbodiimide reagents. These reagents do not cause precipitation even at high loading levels and can be used to efficiently functionalize carboxylic acid coated NPs.
ACS Nano 2009 Apr 28
PMID:Poly(ethylene glycol) carbodiimide coupling reagents for the biological and chemical functionalization of water-soluble nanoparticles. 1927 75

Gold nanorods (AuNRs) are of interest for a wide range of applications, ranging from imaging to molecular electronics, and they have been studied extensively for the past decade. An important issue in AuNR applications is the ability to self-assemble the rods in predictable structures on the nanoscale. We here present a new way to end-to-end link AuNRs with a single or few linker molecules. Whereas methods reported in the literature so far rely on modification of the AuNRs after the synthesis, we here dimerize gold nanoparticle seeds with a water-soluble dithiol-functionalized polyethylene glycol linker and expose the linked seeds to growth conditions identical to the synthesis of unlinked AuNRs. Doing so, we obtain a large fraction of end-to-end linked rods, and transmission electron microscopy provides evidence of a 1-2 nm wide gap between the AuNRs. Flow linear dichroism demonstrates that a large fraction of the rods are flexible around the hinging molecule in solution, as expected for a molecularly linked nanogap. By using excess of gold nanoparticles relative to the linking dithiol molecule, this method can provide a high probability that a single molecule is connecting the two rods. In essence, our methods hence demonstrate the fabrication of a nanostructure with a molecule connected to two nanoelectrodes by bottom-up chemical assembly.
ACS Nano 2009 Apr 28
PMID:Self-assembled nanogaps via seed-mediated growth of end-to-end linked gold nanorods. 1928 31

By means of high-resolution scanning tunneling microscopy (STM), we have revealed unprecedented details about the intermediate steps for a surface-catalyzed reaction. Specifically, we studied the oxidation of H adatoms by O(2) molecules on the rutile TiO(2)(110) surface. O(2) adsorbs and successively reacts with the H adatoms, resulting in the formation of water species. Using time-lapsed STM imaging, we have unraveled the individual reaction intermediates of HO(2), H(2)O(2), and H(3)O(2) stoichiometry and the final reaction product-pairs of water molecules, [H(2)O](2). Because of their different appearance and mobility, these four species are discernible in the time-lapsed STM images. The interpretation of the STM results is corroborated by density functional theory calculations. The presented experimental and theoretical results are discussed with respect to previous reports where other reaction mechanisms have been put forward.
ACS Nano 2009 Mar 24
PMID:Observation of all the intermediate steps of a chemical reaction on an oxide surface by scanning tunneling microscopy. 1930 69

Polymer vesicles with diameters of ca. 100-600 nm and bearing benzaldehyde functionalities within the vesicular walls were constructed through self-assembly of an amphiphilic block copolymer PEO(45)-b-PVBA(26) in water. The reactivity of the benzaldehyde functionalities was verified by cross-linking the polymersomes and also by a one-pot cross-linking and functionalization approach to further render the vesicles fluorescent, each via reductive amination. In vitro studies found these labeled nanostructures to undergo cell association.
ACS Nano 2009 Mar 24
PMID:Benzaldehyde-functionalized polymer vesicles. 1930 73

We have created stable dispersions of single wall carbon nanotubes (SWNTs) in water by employing a noncovalent functionalization scheme that allows carboxylic acid moieties to be attached to the SWNT surface by a pi-pi stacking interaction. Pyrenecarboxylic acid (PCA) is noncovalently attached to the surface of SWNTs and affords highly uniform and stable aqueous dispersions. This method was developed to provide a noncovalent alternative to the commonly used oxidative acid treatment functionalization of carbon nanotubes. This alternative strategy avoids the damage to the carbon nanotube structure inherent to oxidative acid treatments. Carbon nanotubes are commonly functionalized with oxidative acid treatment schemes to create polymer-nanotube composites and improve the adhesion between the polymer and carbon nanotubes. Composites of SWNTs and polycarbonate were prepared and tested to determine the effect of PCA on the adhesion of the SWNTs to the polymer matrix. These tests confirmed that PCA improved the SWNT-polycarbonate adhesion and improved the dispersion of the SWNTs throughout the matrix. This study demonstrates that stable dispersions of SWNTs can be achieved without substantial cutting, introduction of defects, or covalent modification, by employing a simple and effective noncovalent functionalization with PCA.
ACS Nano 2009 Apr 28
PMID:Noncovalent functionalization as an alternative to oxidative acid treatment of single wall carbon nanotubes with applications for polymer composites. 1933 88

We report an industrially scalable, fast, and simple process for the large scale fabrication of optically transparent and electrically conducting thin films of single-walled carbon nanotubes (SWNT). Purified, pristine HiPco SWNTs were dispersed in water at high concentrations with the help of surfactants, rod-coated into uniform thin films, and doped by various acids. We show how to combine different surfactants to make uniform dispersions with high concentration of SWNTs and optimal rheological behavior for coating and drying, including preventing dewetting and film rupture that has plagued earlier attempts. Doping by fuming sulfuric acid yielded the films with best performance (sheet resistance of 100 and 300 Omega/sq for respective transparency of 70% and 90%). We use a figure of merit (FOM) plot for an immediate evaluation and comparison of the performance and microstructure of CNT films produced by different methods. Further scientific engineering will pave the way to the deployment of CNT films in commercial applications.
ACS Nano 2009 Apr 28
PMID:Continuous and scalable fabrication of transparent conducting carbon nanotube films. 1935 79


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