ChemPlusChem

Description

ChemPlusChem is a peer-reviewed journal tailored to multidisciplinary chemistry and materials researchers from across the world. Fully comprehensive in its scope, ChemPlusChem publishes original papers covering at least two different aspects (subfields) of chemistry or one of chemistry and one of another scientific discipline (one chemistry topic plus another one, hence the title ChemPlusChem).

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  • ISSN
    2192-6506

Publications in this journal

  • [Show abstract] [Hide abstract]
    ABSTRACT: A multifunctional floating photocatalyst consisting of highly active well-ordered mesoporous TiO2 (OMT) as a catalyst and polyurethane foam (PUF) as a floating substrate is synthesized successfully through a low-temperature ultrasonic and deposition approach. With the synthesized OMT/PUF composites, the multifunctionality of contaminant adsorption, dye degradation, and heavy metal removal can be achieved simultaneously. The prepared photocatalyst is characterized in detail by X-ray diffraction, Raman spectroscopy, transmission electron microscopy, scanning electron microscopy, and N2 adsorption. The results indicate that the OMT/PUF presents a hierarchical macro/mesoporous structure, which is favorable for the adsorption and diffusion of pollutants and for the efficient utilization of sunlight. The degradation of several model dyes including rhodamine B, methyl orange, methylene blue, and simultaneous reduction of hexavalent chromium are examined over the floating photocatalysts with sunlight irradiation under certain conditions. A synergistic effect between the degradation of dyes and the reduction of CrVI is observed for the dye-CrVI coexistence system. This novel floating OMT/PUF photocatalyst is very promising in the field of wastewater treatment.
    ChemPlusChem 12/2014;
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    ABSTRACT: Host-secreted antimicrobial peptides (AMPs) are found in virtually all organisms, often providing innate immunity as the first line of defence against pathogens. Many AMPs kill pathogens by disrupting their cellular membranes and thus are similar to some antibiotic drugs. Likely drug candidate AMPs are found in non-mammalian hosts but are also haemolytic. Thus, it is crucial to understand the origins of membrane specificity and selectivity of the action of these AMPs. In this study, the membrane specificity of action of citropin 1.1, a 16-residue AMP, was studied by using a quartz crystal microbalance on the basis of mass and viscoelasticity changes in comparison to aurein 1.2 (13 residues) and maculatin 1.1 (21 residues). The membrane selectivity was largely reflected in the nature of the initial interaction of the peptide with the membrane. This initial interaction might determine whether the peptide transforms into a membrane-disrupting α-helical conformation and highlights subtle differences in the repositioning of this α-helical peptide in the membrane, as reflected by the viscoelasticity data, thus signifying the mechanistic pathway to membrane disruption.
    ChemPlusChem 12/2014;
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    ABSTRACT: Porpholactones and their derivatives have attracted increasing attention for their promising application as photosensitizers. Reduction of the β-lactone moiety in porpholactone to β-hemiacetal, named porpholactol, allows the synthesis of chlorin-type photosensitizers with enhanced near-infrared absorption as well as β functionalization of water-soluble conjugates. By employing β-hydrophilic conjugates terminated by different ionic groups, such as neutral (ZnL1), anionic (ZnL2), zwitterionic (ZnL3), and cationic (ZnL4–6) groups, a series of photosensitizers (ZnL1–6) were synthesized and characterized, and their photophysical properties were studied, including magnetic circular dichroism measurement. The terminal ionic groups on β conjugates influence significantly the cellular uptake of ZnL1–6 in the order ZnL4–6 (positive charge)>ZnL1–3 (negative charge or neutral). Importantly, the photocytotoxicity of ZnL1–6 against cancer cells showed IC50 values down to the sub-micromolar range and exhibited the same trend as their cellular uptake, clearly revealing the relationship of β-ionic conjugates, cellular uptake, and intracellular photodynamic therapy (PDT) activity. Furthermore, using ZnL4 as an example, mechanistic studies, such as cell imaging experiments and Western blot analysis for the PDT process, indicate that ZnL4 exerts photodynamic activity through apoptosis, which is highly associated with lysosome disruption, mitochondria depolarization, and nuclei condensation.
    ChemPlusChem 12/2014;
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    ABSTRACT: Targeted delivery provides a means to overcome the systemic toxicity of cancer chemotherapeutics. Maleimide functionalization of anticancer-active metal complexes allows their site-selective covalent conjugation to human serum albumin (HSA) to exploit passive targeting to the tumor site through the enhanced permeability and retention (EPR) effect. By incorporating the maleimide moiety in the monodentate N-donor coligands, a series of [MII(cym)X2] (M=Ru, Os; cym=η6-p-cymene; X=Cl2, Br2, I2, oxalate) complexes was synthesized and characterized. The influence of the metal center, η6-arene, and leaving group X on the chemical and biological properties was studied. The compounds exhibited low stability in dimethyl sulfoxide (DMSO) but were more stable in the 5 % aqueous DMSO solution used in biological assays. Incubation with cysteine as a model for thiol-containing biomolecules demonstrated high reactivity of the maleimide with the thiol group. In in vitro anticancer assays in human colorectal, non-small-cell lung, and cervical carcinoma cells the complexes were good to moderately active with the lowest IC50 value at 8 μM for an osmium–iodido complex.
    ChemPlusChem 12/2014;
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    ABSTRACT: A new bimodal and multivalent dendritic contrast agent (CA) that targets the protein avidin was prepared and characterized. The tripartite lysine core was used to link the ligand biotin, the fluorescent dye, and the dendron carrying GdDOTA (DOTA=1,4,7,10-tetraazacyclododecane-1,4,7,10-tetraacetic acid) chelates for amplification of the magnetic resonance imaging (MRI) signal. The longitudinal relaxivity of this dendrimeric CA was greater than those of its GdDOTA chelate and most of the common commercial agents at the investigated high magnetic field (7 T). The capacity of the dendrimeric CA to bind to the target protein was confirmed by fluorescence measurements upon its treatment with NeutrAvidin–agarose gel or NeutrAvidin-coated microspheres and the results were compared with those of its monomeric analogue. The fluorescence intensity of monomer-treated targets was found to be greater than that from those treated with dendrimeric CA; however, a several-fold increase in the MRI signal was observed on the same samples treated with the dendrimeric CA. The inductively coupled plasma mass spectrometry analysis of the digested samples indicated somewhat higher Gd3+ content and hence slightly better binding of monomeric versus dendrimeric CA. This bimodal and multivalent targeted probe opens an avenue for the preparation of new nanosized CAs that allow high-resolution MRI of various targets, such as cellular receptors or specific cellular populations.
    ChemPlusChem 12/2014;
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    ABSTRACT: GeSe single-crystalline microtubes with a rectangular cross section have been fabricated through a facile solution approach. The as-prepared GeSe microtubes have diameters in the range of 1–2 μm and wall thicknesses of approximately 100–200 nm. Crystal growth along the [010] direction is preferable for the GeSe microtubes. The formation of GeSe microtubes is proposed to originate from an etching effect of the solvent oleylamine. A clear photoresponsive behavior has been found for the as-synthesized GeSe microtubes. The products were characterized by using powder XRD, energy-dispersive X-ray spectroscopy, TEM, SEM, and UV/Vis spectrophotometry.
    ChemPlusChem 12/2014;
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    ABSTRACT: A novel nanoconstruct based on poly(lactic-co-glycolic acid) nanoparticles loaded with a tetrathiahelicene molecule conjugated to a fluorescent rhodamine probe was prepared and characterized. Because helicenes are known to be very promising DNA intercalators, the tetrathiahelicene was selected for this study as a model therapeutic cytotoxic molecule. The ability of the nanoconstruct to internalize the tetrathiahelicene and deliver it intracellularly in a safe manner has been investigated by means of cytotoxicity and cell uptake tests on Balb/3T3 clone A31 fibroblasts. The outcomes of this study suggest the suitability of the developed nanoconstruct to act as a vector for the intracellular delivery of hydrophobic small molecules, such as helicenes, thus contributing to their possible future exploitation as novel therapeutics.
    ChemPlusChem 12/2014;
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    ABSTRACT: A new class of carbazolo[2,1-a]carbazole diimide compounds (CBZCBZ-DI, 3) are designed and synthesized. The synthesis, X-ray crystal structure, absorption spectra, and electrochemical properties of 3 as well as the charge transport properties are investigated. Theoretical calculation is also carried out based on the X-ray crystal structure of 3 a to understand the relationship between the structure and the charge transport properties. Single-crystal X-ray analysis revealed that the molecules of 3 a adopt a slipped face-to-face π-stacking mode with a large intermolecular π-overlap and an interplanar distance of 3.4 Å. Crystalline transistors of 3 a display high hole mobility of 0.5 cm2 V−1 s−1, which is among the highest reported mobility values for carbazole-based N-heteroacenes. Two useful brominated derivatives (4, 5) are also prepared for synthesizing more new π-functional materials.
    ChemPlusChem 12/2014;
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    ABSTRACT: Y2O3:Eu3+ nanoparticles (NPs), polyaniline (PANI), and Fe3O4 NPs are incorporated into polymethyl methacrylate (PMMA) and electrospun into [Y2O3:Eu3+/PMMA]//[PANI/Fe3O4/PMMA] Janus nanobelts with Y2O3:Eu3+/PMMA as one half side and PANI/Fe3O4/PMMA as the other. The morphology and properties of the final products are investigated in detail by X-ray diffraction (XRD), scanning electron microscopy (SEM), optical microscopy (OM), energy-dispersive spectrometry (EDS), Hall effect measurements, fluorescence spectroscopy, vibrating sample magnetometry (VSM), and UV/Vis spectroscopy. The results reveal that the [Y2O3:Eu3+/PMMA]//[PANI/Fe3O4/PMMA] trifunctional Janus nanobelts possess excellent electrical conductivity, magnetism, and fluorescence owing to their special nanostructure. Fluorescence emission peaks of Eu3+ are observed in the Janus nanobelts. The electrical conductivity reaches the order of 10−4 S cm−1. The luminescent intensity, electrical conductivity, and saturation magnetization of the Janus nanobelts can be tuned by adjusting the respective amounts of Y2O3:Eu3+ NPs, PANI, and Fe3O4 NPs. The flexible luminescent-electrical-magnetic trifunctional Janus nanobelts have many potential applications. More importantly, this design concept and construct technology is of universal significance for the fabrication of other multifunctional nanostructures.
    ChemPlusChem 12/2014;
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    ABSTRACT: The synthesis of Zr and Hf twin monomers of type [M(2-OCH2cC4H3O)4(x HOCH2cC4H3O)] (3, M=Zr, x=0; 4, M=Hf, x=1) and M[(2-OCH2-C6H4O)2(2-HOCH2-C6H4OH)] (5, M=Zr; 6, M=Hf) by reacting M(OR)4 (M=Zr, R=nC3H7, 1; M=Hf, R=nC4H9, 2) with 2-furylmethanol or 2-hydroxybenzyl alcohol is discussed. Complexes 3–6 were homopolymerized under acidic conditions. Additionally, 5 and 6 were copolymerized with 2,2′-spirobi[4 H-1,3,2-benzodioxasiline] (SBS). Under acidic conditions SBS forms a phenolic resin/SiO2 nanostructured material. The resulting hybrid materials from the homopolymerization of 3–6 and the copolymerized materials from 5 and 6 were characterized by standard solid-state analytics. The inorganic lattice of the MO2 materials from the homopolymerized complexes 3–6 and SiO2/MO2 from the copolymerization of 5 and 6 with SBS was obtained by air oxidation. The oxide materials were characterized by X-ray powder diffraction (XRPD) and energy-dispersive X-ray analysis, which proved their identity. The inner surface area was determined by N2 adsorption/desorption studies, which revealed surface areas of 100 m2 g−1 for MO2. The mixed oxides SiO2/MO2 were additionally investigated by differential scanning calorimetry and variable-temperature XRPD to study the thermal behavior. It was found that crystallization of tetragonal MO2 nanoparticles is characteristic within the SiO2 matrix, but higher sintering temperatures caused crystallization of the SiO2 lattice.
    ChemPlusChem 12/2014;
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    ABSTRACT: Electrospun carbon fiber electrodes showing high performance for bio-electrochemical applications were developed. Easy to handle and manipulate aligned and unaligned carbon fibers with a mean diameter of (330±50) nm were synthesized through an electrospinning technique. Electrical resistivity measurements, which are a challenge that has not been much explored in the case of fibrous materials, were realized through two different techniques, and a study of contact resistances between electrical clips and the carbon fibers was performed. To target the creation of a bioelectrode, carbon fibers were characterized electrochemically by cyclic voltammetry. After being modified with the enzyme laccase, its response to oxygen electroreduction was studied. Aligned fibers present a cathodic current that is 30 % higher than that of randomly distributed fibers. Overall, the results show that aligned fibers are more appropriate for bio-electrochemical applications when exploiting anisotropic spatial organization.
    ChemPlusChem 11/2014;
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    ABSTRACT: A continuous mixed Fe-W-O thin-films materials library was fabricated by means of reactive co-sputtering from elemental iron and tungsten targets in argon/oxygen. The materials library was screened for its local photoelectrochemical properties by using an automated optical scanning droplet cell. Local scanning electron microscopy (SEM) and electron-dispersive X-ray spectroscopy (EDX) measurements of the materials library were performed to correlate the composition, morphology, and photocurrents. The iron content was varied in the range from Fe32W68Ox to Fe81W19Ox. A strong dependence of the film morphology and the measured photocurrents on the composition was observed with a maximal photocurrent from a measurement area containing 55 at % iron. The most photoactive area showed a porous structure with a high surface area. The bandgap values of these materials were assessed by photocurrent spectroscopy and showed a systematic variation of the bandgap values with the composition.
    ChemPlusChem 11/2014;
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    ABSTRACT: An amino-core-substituted naphthalenediimide (NDI) derivative has been synthesized in good yield in two steps. The NDI bearing a diamine moiety undergoes a reversible protonation–deprotonation process, which results in intensity changes in the absorption and emission spectra. This derivative exhibits good photostability, good selectivity, high sensitivity, and is employed to exhibit the pH within the rough endoplasmic reticulum of living cells.
    ChemPlusChem 11/2014;
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    ABSTRACT: Size exclusion is a widespread phenomenon in supra- and macromolecular chemistry. Herein, the size exclusion properties of polyphenylene dendrimers on the surface of high fundamental frequency quartz crystal microbalances are reported. For this purpose, a new dense fifth-generation polyphenylene dendrimer, which was previously not possible owing to the high steric demand of the dendron arms, was synthesized. By increasing the volume and size of subjected analytes an affinity shift from smaller to larger dendrimers can be obtained.
    ChemPlusChem 11/2014;
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    ABSTRACT: By introducing 2,6-bis(2-benzimidazolyl)pyridyl and 2,6-di-(pyrazol-3-yl)pyridine derivatives as ligand in the reaction system, three new transition-metal coordination complexes have been successfully synthesized, namely, [Co(HL1)2] (1), [Ni(HL1)2] (2), and [Ni3(H2L2)2⋅(HL2)2]⋅(OH)3⋅(Ac)⋅H2O (3) (H2L1=2,6-bis(benzimidazol-2-yl)pyridine and H2L2=2,6-di-(5-phenyl-1H-pyrazol-3-yl)pyridine). They are all characterized by elemental analysis, IR spectroscopy, UV absorption spectroscopy, thermogravimetric analysis, powder X-ray diffraction, and single-crystal X-ray diffraction. Structural analysis shows that the structures of complexes 1 and 2 are similar. They are constructed from one metal (Co, Ni) atom and two 2,6-bis(benzimidazol-2-yl)pyridine ligands (HL1−); the HL1− ligand is in the tridentate coordination mode with N3 donors. Complex 3 is a trinuclear Ni complex with four 2,6-di-(5-phenyl-1H-pyrazol-3-yl)pyridine (H2L2) ligands, in which the H2L2 possesses two coordination fashions: terminal tridentate and bridging tetradentate. In addition, the surface photovoltage spectroscopy and photocatalytic activities of complexes 1–3 were investigated in detail. The results reveal that complex 3 possesses higher photocatalytic activity.
    ChemPlusChem 11/2014;
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    ABSTRACT: Magnesium silicate double-walled hollow nanofibers (MSHNFs) with a hierarchical nanostructure have been successfully fabricated by combining the electrospinning technique with a hydrothermal method. The as-prepared MSHNFs are composed of numerous ultrathin nanosheets with a thickness of approximately 10 nm and have a high specific surface area (632.2 m2 g−1) and large pore volume (0.92 cm3 g−1). The MSHNFs exhibit high adsorption capacity and excellent stability in a purification test with organic molecules and a solution of heavy-metal ions. Moreover, the MSHNFs can be easily separated from solution by gravitational sedimentation owing to their unique structure.
    ChemPlusChem 11/2014;
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    ABSTRACT: The Zn–Ce flow battery is a recently introduced hybrid redox flow battery (RFB) but has been extensively studied in the laboratory and at the industrial pilot scale since its introduction in 2005. The cell has the highest open-circuit cell potentials amongst aqueous RFBs, which can exceed 2.4 V at full charge. Although original patents were filed in 2004 and 2005, the history of the half-cell reactions stretches back many decades, with the CeIV/CeIII redox couple being well studied in sulfuric acid as a redox mediator in organic electrosynthesis or in nitric acid for specialist cleaning in the chemical and nuclear industries; in addition, zinc deposition and stripping in acid media are well known in hydrometallurgy and electroplating of metals as well as in other secondary batteries using zinc negative electrodes. Methanesulfonic acid electrolytes were introduced in surface finishing several decades ago but their use in flow batteries is only 20 years old. This Review considers the thermodynamics and kinetics of the electrode reactions (desired and secondary) in each half-cell, operational variables, materials for cell components, cell design and performance of the zinc–cerium flow battery. Continuing challenges are highlighted and critical research needs for the science and technological development are considered.
    ChemPlusChem 11/2014;
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    ABSTRACT: A facile, eco-friendly method for the synthesis of gold/platinum catalysts through electrodeposition of platinum nanoparticles, followed by the deposition of solutions of HAuCl4 onto the surface of pre-prepared platinum for a galvanic replacement reaction, is reported. Different molar ratios of bimetallic structures of platinum and gold could be easily achieved and characterized by energy-dispersive X-ray spectroscopy, SEM, and XRD. Electrochemical measurements reveal that the electrocatalytic activities of these series of gold/platinum catalysts towards formic acid oxidation reaction are superior to that of pure platinum. In addition, the formic acid oxidation route is related to the molar ratio of gold to platinum, which can be ascribed to the influence of gold. The gold/platinum catalyst with a platinum to gold atomic ratio of 2.51:1 exhibits maximum activity. Moreover, this optimized molar ratio shows a highly stable electrocatalytic activity for CO antipoisoning effects. These experimental results suggest that the prepared gold/platinum catalysts have great potential for applications in fuel cells.
    ChemPlusChem 11/2014;
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    ABSTRACT: Various α-Fe2O3 hollow structures, such as wormlike shapes, ellipsoids, and quasicubes, were synthesized successfully by a halide-ion-assisted solvothermal method. The self-assembly assisted by selective absorption of halide ions and Ostwald ripening speeded up by acidic etching commonly determine the final unique structures. The electrochemical performance of the α-Fe2O3 with different structures in reversible lithium-ion storage was investigated, and showed that the hollow Fe2O3 quasicubes exhibit the best cycling performance with a charge capacity of 401.6 mAh g−1 after 100 cycles at 0.2 C. The superior cycling stability and high specific capacity can be ascribed to the higher specific surface area, lower charge-transfer resistance, and adequate alleviation of volume variation.
    ChemPlusChem 11/2014;
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    ABSTRACT: Folic acid has emerged as an interesting cell-targeting moiety and a number of drugs have been conjugated to folate. In this context, new conjugates of β-cyclodextrins with folate have been synthesised as drug carriers to improve their selectivity for cells overexpressing the folic acid receptor. In particular, both 3- and 6-functionalised β-cyclodextrins, linked to the α- or γ-carboxylic group of folic acid, have been synthesised and fully characterised. As a proof of concept, the antitumour platinum(IV) complex cis–trans–cis-[PtCl2(CH3CO2)2(adamantylamine)(NH3)] (LA-12) has been used as a guest drug. The LA-12–cyclodextrin inclusion complexes have been tested on tumour cells. In the presence of cyclodextrin–folate conjugates, LA-12 exhibited IC50 values four times smaller than those of LA-12 alone in MDA-MB-231 cells, which overexpress folic acid receptors on their membrane. No improvement of LA-12 cytotoxicity was found in control tumour cells that do not overexpress the folate receptor. Thus, the non-covalent approach, based on inclusion complexes with functionalised cyclodextrins, looks very promising for drug targeting.
    ChemPlusChem 11/2014;