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We successfully synthesized hyperbranched poly(triazole)s by in situ click polymerization of diazides 1 and triyne 2 monomers on different metal surfaces (copper, iron, and aluminum) and characterized their adhesive properties. Optimizations were performed to obtain high adhesive strength at different temperatures by analyzing the effects of curing kinetics, annealing temperature and time, catalyst, monomer ratio, surface conditions, alkyl chain length of diazides 1, etc. The adhesive bonding strength with metal substrate is 2 orders of magnitude higher than similar hyperbranched poly(triazole)s made by click polymerization and clearly higher than some commercial adhesives at elevated temperatures. With the same conditions, adhesives prepared on aluminum and iron substrates have higher adhesive strength than those prepared on copper substrate, and an excess of triyne 2 monomer in synthesis has greater adhesive strength than an excess of diazide 1 monomer. Tof-SIMS experiment was employed to understand these phenomena, and the existence of an interphase between the polymer and metal surface was found to be critical for adhesive bonding with thicker interphase (excess of triyne 2 monomer) and the higher binding energy between polymer atoms and substrate atoms (e.g., aluminum substrate) generating the higher bonding strength. In addition, the light-emitting property of synthesized polymers under UV irradiation can be used to check the failure mode of adhesive bonding.
ACS Appl Mater Interfaces 2010 Feb
PMID:Synthesis and curing of hyperbranched poly(triazole)s with click polymerization for improved adhesion strength. 2035 6

A strategy for the rational design of a novel colorimetric sensor based on dithioerythritol-modified gold nanoparticles for the selective recognition of Hg2+ in aqueous media is presented. This approach relies on the combination of gold nanoparticles with Hg2+ through sulfur-Hg2+-sulfur interaction. The gold nanoparticles showed high selectivity toward Hg2+ with binding-induced red shift in the absorption spectra, with no response to major interfering cations such as Pb2+, Cd2+, and Cu2+ in the presence of ethylenediamine tetraacetic acid. The system responds to Hg2+ with a detection limit of 100 nM and might open a new avenue for the development of Hg2+ sensing probes.
ACS Appl Mater Interfaces 2010 Jan
PMID:Highly sensitive gold nanoparticle-based colorimetric sensing of mercury(II) through simple ligand exchange reaction in aqueous media. 2035 48

We present herein efficient bulk heterojunction (BHJ) solar cells via mixing poly[2,7-(9,9-dihexylfluorene)-alt-bithiophene] (F6T2) and 6,6-phenyl C61 butyric acid methyl ester (PCBM) with variable weight ratios. The photo-physics and morphology of F6T2:PCBM blend films and the electrical characteristics of their corresponding single cells were studied in details by changing PCBM concentration. The complete photoluminescence quenching of F6T2 emission occurs with only a small fraction of PCBM blended, demonstrating effective photoinduced charge transfer between F6T2 and PCBM. Morphology images from atomic force microscopy and scanning electron microscopy (SEM) reveal that the phase separation in F6T2:PCBM blend films becomes pronounced with the increase of PCBM concentration, resulting in the increased fill factor from 25.2% (1:1) to 56.9% (1:6). A SEM image also shows the phase separation is within the range of 10 - 20 nm. With the optimized F6T2:PCBM weight ratio (1:2), the single cell exhibits a highest power conversion efficiency of 2.46% due to the balance of light absorption and charge transport. Finally, the polymer-small molecule tandem cells are constructed using F6T2:PCBM BHJ as the bottom cell and copper phthalocyanine (CuPc):fullerene (C(60)) as the top cell. The open-circuit voltage (V(oc)) of tandem cell (1.27 V) is equal to the summation of the V(oc) values of the bottom cell (0.86 V) and the top cell (0.43 V).
ACS Appl Mater Interfaces 2010 Mar
PMID:Efficient bulk heterojunction solar cells with poly[2,7-(9,9-dihexylfluorene)-alt-bithiophene] and 6,6-phenyl C61 butyric acid methyl ester blends and their application in tandem cells. 2035 88

Three imidazolium-based ionic liquids containing sterically hindered phenol groups were synthesized. The cation was 1-(3,5-ditert-butyl-4-hydroxybenzyl)-3-methyl-imidazolium, and the anions were tetrafluoroborates, hexafluorophosphates, and bis(trifluoromethylsulfonyl)imide. The physical properties of the synthetic products and of poly(ethylene glycol) (PEG) with the additive were evaluated. The oxidative stability of 0.5 wt % 1-(3,5-di-tert-butyl-4-hydroxybenzyl)-3-methyl-imidazolium hexafluorophosphates in PEG were assessed via rotating bomb oxidation test (RBOT), thermal analysis, and copper strip test. The tribological behaviors of the additives for PEG application in steel/steel contacts were evaluated on an Optimol SRV-IV oscillating reciprocating friction and wear tester as well as on MRS-1J four-ball testers. The worn steel surface was analyzed by a JSM-5600LV scanning electron microscope and a PHI-5702 multifunctional X-ray photoelectron spectrometer. RBOT test, thermal analysis, and copper strip test results revealed that synthesized ionic liquids possessed excellent antioxidant properties. Tribological application results revealed that these could effectively reduce friction and wear of sliding pairs compared with the PEG films used without the additives. Specifically, (BHT-1)MIMPF(6) exhibited better antiwear properties at an optimum concentration of 1 wt %. At this level, its antiwear property significantly improved by 100 times with respect to using just the PEG base oil. Boundary lubrication films composed of metal fluorides, organic fluorines, organic phosphines, and nitride compounds were formed on the worn surface, which resulted in excellent friction reduction and antiwear performance.
ACS Appl Mater Interfaces 2010 Mar
PMID:Imidazolium ionic liquids as antiwear and antioxidant additive in poly(ethylene glycol) for steel/steel contacts. 2035 93

A new, efficient, palladium- and chromium-free process for the electroless plating of acrylonitrile-butadiene-styrene (ABS) polymers has been developed. The process is based on the ion-exchange properties of poly(acrylic acid) (PAA) chemically grafted onto ABS via a simple and one-step method that prevents using classical surface conditioning. Hence, ABS electroless plating can be obtained in three steps, namely: (i) the grafting of PAA onto ABS, (ii) the copper Cu(0) seeding of the ABS surface, and (iii) the nickel or copper metallization using commercial-like electroless plating bath. IR, XPS, and SEM were used to characterize each step of the process, and the Cu loading was quantified by atomic absorption spectroscopy. This process successfully compares with the commercial one based on chromic acid etching and palladium-based seed layer, because the final metallic layer showed excellent adhesion with the ABS substrate.
ACS Appl Mater Interfaces 2010 Apr
PMID:ABS polymer electroless plating through a one-step poly(acrylic acid) covalent grafting. 2036 51

We report the implementation of continuous, highly flexible, and transparent graphene films obtained by chemical vapor deposition (CVD) as transparent conductive electrodes (TCE) in organic photovoltaic cells. Graphene films were synthesized by CVD, transferred to transparent substrates, and evaluated in organic solar cell heterojunctions (TCE/poly-3,4-ethylenedioxythiophene:poly styrenesulfonate (PEDOT:PSS)/copper phthalocyanine/fullerene/bathocuproine/aluminum). Key to our success is the continuous nature of the CVD graphene films, which led to minimal surface roughness ( approximately 0.9 nm) and offered sheet resistance down to 230 Omega/sq (at 72% transparency), much lower than stacked graphene flakes at similar transparency. In addition, solar cells with CVD graphene and indium tin oxide (ITO) electrodes were fabricated side-by-side on flexible polyethylene terephthalate (PET) substrates and were confirmed to offer comparable performance, with power conversion efficiencies (eta) of 1.18 and 1.27%, respectively. Furthermore, CVD graphene solar cells demonstrated outstanding capability to operate under bending conditions up to 138 degrees , whereas the ITO-based devices displayed cracks and irreversible failure under bending of 60 degrees . Our work indicates the great potential of CVD graphene films for flexible photovoltaic applications.
ACS Nano 2010 May 25
PMID:Continuous, highly flexible, and transparent graphene films by chemical vapor deposition for organic photovoltaics. 2039 55

An electrochromic-type electronic paper was prepared using nanocomposites that consisted of silica nanoparticles (silica 60 wt %) and polyamide pulp. Its light scattering, ion transport, and aqueous electrolyte retention characteristics were examined. As a result, the shape of the nanocomposites was completely self-standing, though it could be impregnated with about nine times as much water on a weight basis. Moreover, its light scattering property was extremely similar to paper. Because of the impregnation of a large amount of water, the ion transport property of the nanocomposites was the same as that of the electrolyte solution without the nanocomposites. The nanocomposites was impregnated using an aqueous solution in which bismuthyl perchlorate (redox species), copper perchlorate, perchloric acid, sodium perchlorate, hydroquinone (electron mediator) and 2-buthyne-1,4-diol (leveling agent) were dissolved. The electronic paper was then prepared by sandwiching the nanocomposites between an indium-tin-oxide transparent electrode and a copper sheet. This electronic paper utilizes the reversible codeposition reaction of black Bi-Cu from bismuthyl perchlorate and copper(II) ions. The characteristics of this electronic paper were examined, and excellent characteristics with a white reflectivity of 65%, black reflectivity of 6.4%, contrast ratio of 10:1, operating life of over 1 x 10(6) cycles and open-circuit memory of at least 1 month were obtained. In addition, its driving voltage was 1.2 V, and the write time was 500 ms.
ACS Appl Mater Interfaces 2010 May
PMID:Bismuth electrochromic device with high paper-like quality and high performances. 2040 85

Integrating low dielectric permittivity (low-k) polymers to metals is an exacting fundamental challenge because poor bonding between low-polarizability moieties and metals precludes good interfacial adhesion. Conventional adhesion-enhancing methods such as using intermediary layers are unsuitable for engineering polymer/metal interfaces for many applications because of the collateral increase in dielectric permittivity. Here, we demonstrate a completely new approach without surface treatments or intermediary layers to obtain an excellent interfacial fracture toughness of >13 J/m(2) in a model system comprising copper and a cross-linked polycarbosilane with k approximately 2.7 obtained by curing a cyclolinear polycarbosilane in air. Our results suggest that interfacial oxygen catalyzed molecular ring-opening and anchoring of the opened ring moieties of the polymer to copper is the main toughening mechanism. This novel approach of realizing adherent low-k polymer/metal structures without intermediary layers by activating metal-anchoring polymer moieties at the interface could be adapted for applications such as device wiring and packaging, and laminates and composites.
ACS Appl Mater Interfaces 2010 May
PMID:Ring-opening-induced toughening of a low-permittivity polymer-metal interface. 2041 22

ZnO nanostructures were deposited on flexible polymer sheet and cotton fabrics at room temperature by activated reactive evaporation. Room-temperature photoluminescence spectrum of ZnO nanostructured film exhibited a week intrinsic UV emission and a strong broad yellow-orange visible emission. TEM and HRTEM studies show that the grown nanostructures are crystalline in nature and their growth direction was identified to be along [002]. ZnO nanostructures grown on the copper-coated flexible polymer sheets exhibited stable field-emission characteristics with a threshold voltage of 2.74 V/mum (250 muA) and a very large field enhancement factor (beta) of 23,213. Cotton fabric coated with ZnO nanostructures show an excellent antimicrobial activity against Staphylococcus aureus bacteria (Gram positive), and approximately 73% reduction in the bacterial population is achieved compared to uncoated fabrics after 4 h in viability. Using a shadow mask technique, we also selectively deposited the nanostructures at room temperature on polymer substrates.
ACS Appl Mater Interfaces 2010 Apr
PMID:Optical, field-emission, and antimicrobial properties of ZnO nanostructured films deposited at room temperature by activated reactive evaporation. 2042 21

We present a novel binder-free multiwall carbon nanotube (MWCNT) structure as an anode in Li ion batteries. The interface-controlled MWCNT structure, synthesized through a two-step process of catalyst deposition and chemical vapor deposition (CVD) and directly grown on a copper current collector, showed very high specific capacity, almost three times as that of graphite, excellent rate capability even at a charging/discharging rate of 3 C, and no capacity degradation up to 50 cycles. Significantly enhanced properties of this anode could be related to high Li ion intercalation on the carbon nanotube walls, strong bonding with the substrate, and excellent conductivity.
ACS Nano 2010 Jun 22
PMID:High capacity and excellent stability of lithium ion battery anode using interface-controlled binder-free multiwall carbon nanotubes grown on copper. 2044 Nov 85


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