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We report colloidal quantum dot (CQDs) photovoltaics having a approximately 930 nm bandgap. The devices exhibit AM1.5G power conversion efficiencies in excess of 2%. Remarkably, the devices are stable in air under many tens of hours of solar illumination without the need for encapsulation. We explore herein the origins of this orders-of-magnitude improvement in air stability compared to larger PbS dots. We find that small and large dots form dramatically different oxidation products, with small dots forming lead sulfite primarily and large dots, lead sulfate. The lead sulfite produced on small dots results in shallow electron traps that are compatible with excellent device performance; whereas the sulfates formed on large dots lead to deep traps, midgap recombination, and consequent catastrophic loss of performance. We propose and offer evidence in support of an explanation based on the high rate of oxidation of sulfur-rich surfaces preponderant in highly faceted large-diameter PbS colloidal quantum dots.
ACS Nano 2010 Feb 23
PMID:Quantum dot photovoltaics in the extreme quantum confinement regime: the surface-chemical origins of exceptional air- and light-stability. 2010 59

The use of nanobubbles, the common surfactant sodium dodecyl sulfate (SDS), and nanobubbles in combination with SDS as cleaning agents to remove lysozyme from the solid-liquid interface has been investigated using a quartz crystal microbalance on both hydrophobic and hydrophilic surfaces. On the hydrophobic surface, significant amounts of protein remained on the surface after 10 cycles of nanobubble treatment for 10 s periods in phosphate buffer. The cleaning efficiency of SDS was far superior and was shown to remove approximately 90% of the protein. The use of nanobubbles in combination with SDS failed to improve the cleaning efficiency further. On the other hand, lysozyme on the hydrophilic surface cannot be removed effectively by either 10 cycles of cleaning with nanobubbles or 10 cycles of cleaning with SDS. Nevertheless, the protein can be removed completely after 6 cycles of cleaning with nanobubbles in combination with SDS.
ACS Appl Mater Interfaces 2009 Feb
PMID:Improved cleaning of hydrophilic protein-coated surfaces using the combination of Nanobubbles and SDS. 2035 40

The biocompatibility of iron-polysaccharide complexes has been well-documented. Herein, a stable thrombo-resistant coating was fabricated by consecutive adsorption of Fe (III) and polysaccharides including heparin (Hep) and dextran sulfate (DS) onto various surface by layer-by-layer self-assembly technique via both electrostatic interaction and chemical complexation process. The absorbance at 350 nm increased linearly with the number of Fe3+/Hep multilayer, indicating the formation of multilayer structure and the uniform coating. Compared with (Fe3+/Hep)10, the (Fe3+/DS/Fe3+/Hep)5 coating was more hydrophilic and stable due to the incorporation of DS. The activated partial thromboplastin time (APTT) and platelet adhesion assays showed that both (Fe3+/Hep)10 and (Fe3+/DS/Fe3+/Hep)5 coated surfaces were anticoagulant. The complexing with ferric ions did not compromise the catalytic capacity of heparin to promote antithrombin(III)-mediated thrombin inactivation. Chromogenic assays for heparin activity proved definitively that the inhibition of locally produced thrombin was contributed to the thromboresistance of the surface-bound heparin. The surface with Hep or DS as the outmost layer showed stronger anticoagulant activity than Fe3+, indicating that the outermost layer of the coating played a key role in anticoagulant activity. The utilization of dextran sulfate/heparin surfaces was more advantageous than merely the heparin surface for improving blood-contacting medical devices for long-term usage.
ACS Appl Mater Interfaces 2009 Jan
PMID:Novel thrombo-resistant coating based on iron-polysaccharide complex multilayers. 2035 62

Nuclear magnetic resonance was used to probe the distribution of water and ionic species in a microstructured poly(methyl methacrylate) (PMMA) polymer optical fiber (MPOF), with a plan to assess the suitability of these fibers for aqueous chemosensing. The NMR spectra and the measurements of proton spin relaxation in hydrated fibers demonstrated the presence of two distinct pools of water: water residing in the microstructure channels and the hydration water residing in the polymer matrix of the fiber. No facile chemical exchange between these two pools was present. The NMR peaks of the two pools of water were separated by 1.53 ppm. Relaxation measurements of the fiber samples doped with aqueous copper sulfate showed that charged ions freely entered the microstructure channels but were completely excluded from the polymer matrix of the fiber. Measurements of the apparent diffusion coefficient of water along the axial direction of the fiber showed that water molecules moved unimpeded along the channels. This is the first reported magnetic-resonance study of microstructured optical fibers. The findings suggest that microstructured PMMA fibers are compatible with ionic aqueous solutions and could provide a robust and durable platform for chemical-sensing applications.
ACS Appl Mater Interfaces 2009 Jan
PMID:Magnetic-resonance evaluation of the suitability of microstructured polymer optical fibers as sensors for ionic aqueous solutions. 2035 72

Seeding polymer substrates for the attachment and growth of metallic contacts is an important problem in modern microcircuit fabrication. A new method to effect such polymer metallization is described in which the polymer is first treated with vapor of zirconium or titanium tetra-tert-butoxide and then thermalyzed to give several monolayers of zirconium or titanium oxides that are attached to the polymer surfaces. The thickness of this layer can be controlled by the vapor exposure time. The thin oxide layers withstand removal by strenuous flexing of the polymers, and they absorb copper sulfate from an aqueous solution. Upon simple treatment with dialkylaminoborane or sodium borohydride, the polymer is metallized with copper. The tetra-tert-butoxides can be deposited through a mask, and patterned metallization of the polymers is easily accomplished.
ACS Appl Mater Interfaces 2009 Oct
PMID:A nanoscale metal alkoxide/oxide adhesion layer enables spatially controlled metallization of polymer surfaces. 2035 44

Core/shell nanostructures of polystyrene (PS)/CeO2 have been prepared on conductive glass substrates by using a novel electrochemical route consisting of (i) the electrophoretic deposition of a PS sphere monolayer on the substrate and (ii) the following potentiostatic electrodeposition of CeO2 on the PS sphere template in Ce(NO3)3 aqueous solutions. The structural morphologies of the deposit changed drastically depending on the Ce(NO3)3 concentration; i.e., spherical and needlelike shells were deposited. The deposit was formed only on the PS sphere surface because of an interaction between cationic cerium species and a sulfate group that was immobilized on the PS sphere surface. The spherical shell layer was assigned as CeO2, and the needlelike shells were composed of Ce(OH)3 needles formed on the CeO2 layer surface, indicating that the deposit species changes from CeO2 to Ce(OH)3 during electrodeposition only in a 1 mM Ce3+ solution. Deposition of Ce(OH)3 would begin when electrogenerated hydrogen peroxide was consumed by decomposition under reductive conditions and could no longer oxidize Ce3+ ions. The corresponding CeO2 hollow shells were obtained by thermal elimination of the PS sphere core and transformation of Ce(OH)3 into CeO2 while keeping their original shapes.
ACS Appl Mater Interfaces 2009 May
PMID:Preparation of core/shell and hollow nanostructures of cerium oxide by electrodeposition on a polystyrene sphere template. 2035 93

Mixtures of cationic guar (cat-guar) or cationic hydroxyethylcellulose (cat-HEC) with the anionic surfactants sodium dodecyl sulfate or sodium lauryl ether-3 sulfate have been investigated by a wide range of complementary techniques (phase studies, turbidity measurements, dynamic light scattering, gel-swelling experiments, and in situ null ellipsometry), with the following objectives in mind: (1) to establish the relationship between the bulk phase behavior (precipitation and redissolution) of the polyion/surfactant ion complexes and formation/deposition of such complexes at silica surfaces and (2) to obtain molecular interpretations of the large, previously unresolved, quantitative differences between the various investigated mixtures. There were clear similarities, for each studied system, between the bulk phase behavior, gel swelling, and surface deposition on increasing surfactant concentration. This is because all phenomena reflect the polyion/surfactant ion binding isotherm: an initial binding step at a low critical association concentration (cac) of the surfactant and a second more-or-less cooperative binding step beginning at a second cac, the cac(2). The details of the interactions are system-specific, however, and cat-guar/surfactant mixtures generally had larger precipitation regions and gave rise to larger adsorbed amounts on silica compared to mixtures with cat-HEC of a similar charge density. The observed quantitative differences are attributed to a difference in the hydrophobicity of the polyions. For cat-guar, the comparatively weak hydrophobic polyion/surfactant attraction is seen as a very gradual binding commencing at the cac(2) and continuing past the bulk critical micelle concentration of the surfactant, resulting in an unusually large phase-separation region. For cat-HEC, the dissolution of the precipitate takes place at lower surfactant concentrations because of a stronger hydrophobic interaction between the surfactant and the polyion. The results have implications for the successful design of oppositely charged polyelectrolyte/surfactant formulations for surface deposition applications.
ACS Appl Mater Interfaces 2009 Nov
PMID:Surface deposition and phase behavior of oppositely charged polyion/surfactant ion complexes. 1. Cationic guar versus cationic hydroxyethylcellulose in mixtures with anionic surfactants. 2035 12

An environmentally benign route for the single-step synthesis of mesoporous sulfated titania is described by a seeding method using titanium oxysulfate as the titania source. The hydrolysis was performed in the presence of NaOH and seed under constant-volume conditions around 98 degrees C. The XPS and DRIFT spectra show the existence of a bridged bidentate sulfate complex on the surface of titania. The elimination of sulfur on heat treatment showed a characteristic change in mesoporosity, specific surface area, and crystallinity of the material. The transformation of sulfated titania to anatase was incomplete at 900 degrees C, showing a delay in crystallization due to the presence of sulfur. Studies on the thermal stability of the sulfated titania showed that the material obtained can be used for various applications at temperatures below 300 degrees C. The ammonia-TPD and catalytic performance studies of the sulfated titania samples showed the presence of strong acid sites.
ACS Appl Mater Interfaces 2009 Nov
PMID:Single-step synthesis and structural study of mesoporous sulfated titania nanopowder by a controlled hydrolysis process. 2035 15

Chiral polyelectrolyte multilayers (PEMs) consisting of poly(l-lysine) (PLL), poly(N-(S)alkylated 4-vinylpyridinium iodide), or poly(ethyleneimine maltose) (PEI-m) as polycations and poly(styrenesulfonic acid) sodium salt (PSS) or poly(vinyl sulfate) as polyanions, as well as a nonchiral PEM composed of poly(ethyleneimine) (PEI) and PSS were deposited on silicon substrates and poly(tetrafluoroethylene) membranes using the layer-by-layer method. For these PEMs, enantiospecific interaction toward one enantiomer of either l/d-glutamic acid (l/d-GLU), l/d-tryptophan, or l/d-ascorbic acid (l/d-ASC), respectively, was studied under variation of the concentration, pH, and ionic strength. Both deposition and enantiospecific interaction were analyzed by attenuated total reflection Fourier transform infrared spectroscopy. Our results show a significant enantiospecific preference of d-GLU over l-GLU at PEMs containing PLL and of d-ASC over l-ASC at PEMs containing PEI-m. No such enantiospecific preference was found for nonchiral PEMs containing PEI. The enantiospecificity of PEMs of PLL/PSS toward l/d-GLU could be significantly influenced by the ionic strength and pH values, so that increasing attractive electrostatic interactions resulted in higher enantiospecificity.
ACS Appl Mater Interfaces 2009 Dec
PMID:In situ ATR-FTIR investigation on the preparation and enantiospecificity of chiral polyelectrolyte multilayers. 2035 70

Stimuli-responsive surfaces grafted with thermoresponsive polymers switch from hydrophilic to hydrophobic thermally, making these surfaces attractive in applications such as in microfluidics devices, as antifouling surfaces, and in cell culture and tissue engineering. These materials exhibit changes in wettability as the polymer undergoes a phase transition above its lower critical solution temperature (LCST). Because the presence of salts affects LCSTs in accordance to the Hofmeister series, salt effects on the wettability of these thermoresponsive surfaces will dramatically impact device performance. Prior studies of such effects have focused on the influence of anions. Detailed studies of the effects of cations have not been carried out. Here, the influence of varying cation identity in a series of mono-, di-, and trivalent sulfate salts on the wettability of a stimuli-responsive grafted surface was investigated by measuring advancing water contact angle (Theta(a)) changes. The cation-induced changes in Theta(a) were correlated with corresponding changes in surface morphology examined by AFM. The results showed that the effects of varying cations on surface wettability are as large as the effects of varying anion identity and concentration (i.e., Theta(a) changes of up to 90 degrees). Parallel studies of the effects of varying the cation identity and concentration for these same cation sulfate salts in solution show that cation variation also has a large effect on the LCST of PNIPAM, the stimuli responsive polymer component of the nanocomposite grafts that were studied. Moreover, analyses of the Theta(a) and LCST data using activity showed that the Theta(a) or LCST versus cation activity/concentration could be readily grouped by charge. Such differences are not seen in similar studies where anion identity, charge, and concentration are changed.
ACS Appl Mater Interfaces 2010 Feb
PMID:Parallel effects of cations on PNIPAM graft wettability and PNIPAM solubility. 2035 91


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