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  • Oxazolium iodide modified perovskites for solar cell fabrication
    ChemPlusChem (IF 2.797) Pub Date : 2018-01-18
    Manuel Salado, Erfan Shirzadi, Samrana Kazim, Fei Zhaofu, M K Nazeeruddin, Paul J Dyson, Shahzada Ahmad

    Perovskites solar cells are gaining interest due to their attractive solar-to-electricity conversion efficiencies, although they suffer from certain problems, such as sub-optimal ion migration and stability issues. We studied the inclusion of a phenyloxazolium salt (2-phenyl-3-methyl-oxazolium iodide) in methyl ammonium lead triiodide (MAPbI3) based perovskite solar cells. The fabricated solar cells, not only gave improved photovoltaic properties, but importantly the oxazolium cation can protect the perovskite layers from UV exposure as it down-converts electromagnetic irradiation, i.e. the photons are absorbed in UV and re-emitted at different wavelength. The loading of 2-phenyl-3-methyloxazolium iodide in the perovskite precursor solution was optimized, the resulting perovskite films characterized, and the solar cells fabricated from them evaluated for their performance. Overall, this simple approach to facilitate the optimization of the performance parameters of perovskites films for solar cell applications.

    更新日期:2018-01-18
  • Synthesis of Nontoxic Protoflavone Derivatives through Selective Continuous-Flow Hydrogenation of the Flavonoid B-Ring
    ChemPlusChem (IF 2.797) Pub Date : 2018-01-15
    Sándor B. Ötvös, Máté Vágvölgyi, Gábor Girst, Ching-Ying Kuo, Hui-Chun Wang, Ferenc Fülöp, Attila Hunyadi
    更新日期:2018-01-15
  • Synthesis of Nontoxic Protoflavone Derivatives through Selective Continuous-Flow Hydrogenation of the Flavonoid B-Ring
    ChemPlusChem (IF 2.797) Pub Date : 2018-01-15
    Sándor B. Ötvös, Máté Vágvölgyi, Gábor Girst, Ching-Ying Kuo, Hui-Chun Wang, Ferenc Fülöp, Attila Hunyadi
    更新日期:2018-01-15
  • Trifluoroethoxy-Coated Subphthalocyanines Attract Small Arenes in Their π-Concave Cavity
    ChemPlusChem (IF 2.797) Pub Date : 2018-01-15
    Satoru Mori, Jiandong Wang, Etsuko Tokunaga, Motoo Shiro, Takashi Matsumoto, Seiji Tsuzuki, Norio Shibata
    更新日期:2018-01-15
  • Trifluoroethoxy-Coated Subphthalocyanines Attract Small Arenes in Their π-Concave Cavity
    ChemPlusChem (IF 2.797) Pub Date : 2018-01-15
    Satoru Mori, Jiandong Wang, Etsuko Tokunaga, Motoo Shiro, Takashi Matsumoto, Seiji Tsuzuki, Norio Shibata
    更新日期:2018-01-15
  • Theoretical studies of singlet fission: searching for materials and exploring mechanisms.
    ChemPlusChem (IF 2.797) Pub Date : 2018-01-11
    Achini Japahuge, Tao Zeng

    In this review article, a survey is given for theoretical studies in the subject of singlet fission. Singlet fission converts one singlet exciton to two triplet excitons. With the doubled number of excitons and the longer lifetime of the triplets, singlet fission provides an avenue to improve the photoelectric conversion efficiency in organic photovoltaic devices. It has been a subject of intense research in the past decade. Theoretical studies play an essential role in understanding singlet fission. In this paper, we review theoretical studies in singlet fission since 2006, the year when the research interest in this subject was reignited. Both electronic structure and dynamics studies are covered. Electronic structure studies provided guidelines for designing singlet fission chromophores and insights into the couplings between single- and multi-excitonic states. The latter gives us fundamental knowledge for engineering inter-chromophore conformation to enhance the fission efficiency. Dynamics studies reveal the importance of vibronic couplings in singlet fission.

    更新日期:2018-01-11
  • Morphology independent efficient singlet exciton fission in perylenediimide thin films
    ChemPlusChem (IF 2.797) Pub Date : 2018-01-10
    Yaroslav V. Aulin, Kevin M. Felter, Deniz Gunbas, Rajeev K Dubey, Wolter F. Jager, Ferdinand Grozema

    Perylene diimides are conjugated chromophores that are of considerable interest due to their ability to transform a singlet excited state into two triplets by singlet fission. While singlet fission has previously been reported for certain perylene diimide derivatives there is some uncertainty on the rates and yield of the process in these materials. In this report, we use ultrafast transient absorption spectroscopy, to demonstrate that singlet fission in perylene diimides can occur on a sub-picosecond time scale with quantum yields approaching the theoretical limit of 200%.

    更新日期:2018-01-10
  • CF3 Substitution of [Cu(P^P)(bpy)][PF6] complexes: Effects on Photophysical Properties and Light-emitting Electrochemical Cell Performance
    ChemPlusChem (IF 2.797) Pub Date : 2018-01-09
    Catherine E. Housecroft, Sarah Keller, Fabian Brunner, José M. Junquera, Antonio Pertegás, Maria-Grazia La-Placa, Alessandro Prescimone, Edwin C. Constable, Henk J. Bolink, Enrique Ortí

    We report [Cu(P^P)(N^N)][PF6] complexes with P^P = bis(2-(diphenylphosphino)phenyl)ether (POP) or 4,5-bis(diphenylphosphino)-9,9-dimethylxanthene (xantphos), N^N = CF3-substituted 2,2'-bipyridines (6,6'-(CF3)2bpy, 6-CF3bpy, 5,5'-(CF3)2bpy, 4,4'-(CF3)2bpy, 6,6'-Me2-4,4'-(CF3)2bpy). We present the effects of CF3 substitution on structures, and electrochemical and photophysical properties. The HOMO-LUMO gap is tuned by the N^N ligand; the largest redshift in the MLCT band is for [Cu(P^P)(5,5'-(CF3)2bpy)][PF6]. In solution, the compounds are weak yellow to red emitters. The emission properties depend on the substitution pattern but this cannot be explained by simple electronic arguments. For powders, [Cu(xantphos)(4,4'-(CF3)2bpy)][PF6] has the highest PLQY (50.3%) with an emission lifetime of 12 µs. Compared to 298 K solution behaviour, excited state lifetimes lengthen in frozen Me-THF (77 K) indicating thermally activated delayed fluorescence (TADF). TD-DFT calculations show that the energy gap between the lowest-energy singlet and triplet excited states (0.12-0.20 eV) permits TADF. LECs with [Cu(POP)(6-CF3bpy)][PF6], [Cu(xantphos)(6-CF3bpy)][PF6] or [Cu(xantphos)(6,6'-Me2-4,4'-(CF3)2bpy)][PF6] emit yellow electroluminescence. A LEC with [Cu(xantphos)(6,6'-Me2-4,4'-(CF3)2bpy)][PF6] had the fastest turn-on time (8 min); the LEC with the longest lifetime (t1/2 = 31 h) contained [Cu(xantphos)(6-CF3bpy)][PF6]; these LECs reached maximum luminances of 131 and 109 cd m-2

    更新日期:2018-01-09
  • Boosting the NMR assignment of carbohydrates with clean in-phase correlation experiments
    ChemPlusChem (IF 2.797) Pub Date : 2018-01-06
    Tamás Gyöngyösi, István Timári, Jens Haller, Martin R.M. Koos, Burkhard Luy, Katalin E. Kövér

    We report novel CLIP-COSY based homo- and heteronuclear correlation experiments for the rapid, semi-automated NMR assignment of small-to-medium-sized molecules. The homonuclear CLIP-COSY and corresponding relayed experiments employ the perfect-echo based mixing sequence for in-phase coherence transfer between directly and/or indirectly coupled proton spins. The combined analysis of the resulting CLIP-COSY and relayed spectra allows to easily track down layer by layer the proton-proton connectivity network. In larger molecular structures the narrow chemical shift range of protons may, however, compromise the efficacy of the homonuclear correlation based assignment strategy. To overcome this inherent limitation, we have devised an HSQC-variant of the CLIP-COSY experiment that takes advantage of the larger chemical shift range of the heteronucleus. We demonstrate that combined treatment of HSQC-CLIP-COSY(-relayed) and standard HSQC spectra facilitates simultaneous and semi-automatic assignment of 1H and 13C resonances of medium-sized molecules, such as pentasaccharides. Besides, the recently introduced PSYCHE broadband homonuclear decoupling scheme has been also implemented into the devised homo- and heteronuclear CLIP-COSY based experiments, resulting in fully decoupled high resolution pure-shift correlation spectra.

    更新日期:2018-01-07
  • Engineering biocompatible scaffolds through the design of elastin-based short peptides
    ChemPlusChem (IF 2.797) Pub Date : 2018-01-04
    Md. Musfizur Hassan, Adam D Martin, Pall Thordarson

    A small library of short peptides is synthesized based around the repeat tetrapeptide sequence Gly-Val-Ala-Pro (GVAP) which is found in the hydrophobic domain of tropoelastin. Of the five peptides synthesized, four formed self-supporting hydrogels, with similar secondary structures. The ability to tune the mechanical properties of the resultant hydrogels is demonstrated, and this is understood in relation to fiber bundling. Finally, the cytotoxicity of these elastin-based short peptide hydrogels towards HeLa cells is assessed, with clear evidence that increased aromaticity of the peptide is detrimental towards cell viability.

    更新日期:2018-01-04
  • Solution processed warm white organic light-emitting diodes based on a blue thermally activated delayed fluorescent dendrimer
    ChemPlusChem (IF 2.797) Pub Date : 2018-01-01
    Lu Li, Xiaoqing Liao, Xin Yang, Jiang Cheng, Ying Li, Xiang Meng, Jie Li, Qibing Pei

    Thermally activated delayed fluorescence (TADF) emitters have received much attention for the fabrication of white organic light emitting diodes (WOLEDs); however, the challenge remains in terms of severe efficiency roll off, poor color stability, as well as high cost. In this contribution, solution processed hybrid WOLEDs were obtained by employing a blue TADF dendrimer bis(4-(3,6-bis(3,6-di-tert-butylcarbazol-N-yl) carbazole) phenyl)sulfone (BPS), combined with an orange iridium complex (bis(2-phenylbenzothiazolato) (acetylacetonate)iridium(III)) (Ir(bt)2(acac)) as a co-dopant. The devices achieved a maximum external quantum efficiency of 6.59% and a maximum current efficiency of 17.34 cd/A. The results suggest that the TADF dendrimer as an assistant dopant was helpful to reduce the triplet populations by up-converting the triplet excitons to the singlet state and immediately transferring to Ir(bt)2(acac) by virtue of the long-range Förster resonance energy transfer, thus significantly decreasing the triplet-triplet annihilation (TTA). Moreover, the emitters can act as shallow trapping centers to decrease charge and exciton aggregation. The resulting OLEDs exhibit stable electroluminescent spectra and low efficiency roll-off at relatively high current density. The CIE coordinates (Δ(x, y) varies only by (0.02, 0.02) in the luminance range of 100 to 10,000 cd/m2.

    更新日期:2018-01-02
  • 3D Micropatterned all Flexible Microfluidic Platform for Microwave Assisted Flow Organic Synthesis (MAFOS)
    ChemPlusChem (IF 2.797) Pub Date : 2017-12-27
    Deniz Hur, Mehmet Girayhan Say, Sibel Emir Diltemiz, Fatma Duman, Arzu Ersöz, Rıdvan Say

    In present work, we fabricate large area, all flexible and microwaveable PDMS microfluidic reactor that is printed via 3D bioplotter system. The sacrificial microchannels are printed on Polydimethoxylane (PDMS) substrates by direct ink writing method using water soluble Pluronic F-127 ink and encapsulated between PDMS layers. The structure of micrometer sized channels is analyzed by optical and electron microscopy techniques. The fabricated flexible microfluidic reactors are utilized for acetylation of different amines under microwave irradiation to get acetylamides in shorter reaction time and good yields in Microwave Assisted Flow Organic Synthesis (MAFOS).

    更新日期:2017-12-27
  • Stable Lithium Storage in N-Doped Carbon-Coated Ferric Oxide Yolk-Shell Nanospindles with Preserved Hollow Space
    ChemPlusChem (IF 2.797) Pub Date : 2017-12-21
    Bao-Lin Zhang, Sen Xin, Haili Qin, Huai-Ping Cong, Shu-Hong Yu

    Iron oxide (Fe2O3) is a promising anode material for the next-generation high-energy lithium ion batteries owing to its high theoretical specific capacity, yet suffers from an unstable electrochemistry as represented by a significant volume variation upon (de)lithiation and unstable solid electrolyte interface. Targeting at the above issues, we have developed a double coating synthetic route to prepare a yolk-shell-structured γ-Fe2O3/nitrogen-doped carbon composite, in which spindle-like γ-Fe2O3 cores are encapsulated in the highly conductive carbon shell. Through precisely controlling the void space between the γ-Fe2O3 core and the carbon shell, the volume variation of γ-Fe2O3 during (de)lithiation is well accommodated while the composite still maintains an intact and relatively dense structure, which stabilizes the solid electrolyte interface and is beneficial for improving the practical energy density of material. With a stabilized (de)lithiation electrochemistry and a synergistic storage effect between the two active components, the composite enables excellent Li storage performance in terms of reversible capacity, cycling ability and rate capability.

    更新日期:2017-12-21
  • An H2S-sensing/CO-releasing flavonol that operates via logic gates
    ChemPlusChem (IF 2.797) Pub Date : 2017-12-13
    Tatiana Soboleva, Abby Benninghoff, Lisa M Berreau

    Signaling molecules, including H2S and CO, are involved in a complex interplay within cells to maintain cellular homeostasis. In order to investigate the intracellular interplay of different gasotransmitters, new molecular tools are needed that combine sensing and release capabilities of different small molecules in a single, multifunctional, and highly-regulated molecular platform. Herein, we report the first example of a combined H2S sensor/CO-releasing molecule. We demonstrate that this flavonol-based molecular tool operates intracellularly via a highly regulated AND logic gated input-output sequence and provides fluorescent feedback for the H2S detection and CO release steps. We demonstrate that this linear sequence can be combined with a fluorescent molecular sensor for CO detection via a third distinct emission. Overall, this is the first molecular framework that can combine the sensing of H2S with the controlled release of CO, two gaseous molecules that are known to exhibit reciprocal regulation and have overlapping targets in cellular environments.

    更新日期:2017-12-13
  • Ionic liquids as "masking" solvents on the relative strength of bases in proton transfer reactions.
    ChemPlusChem (IF 2.797) Pub Date : 2017-12-13
    Romina Zappacosta, Antonello Di Crescenzo, Valeria Ettorre, Antonella Fontana, Marco Pierini, Gabriella Siani

    Equilibrium constants for the proton transfer reaction between pyridines and trifluoroacetic acid have been measured in some room temperature ionic liquids (ILs) of different cation-anion compositions. The experimental equilibrium constant for ion pair formation have been corrected according to the Fuoss equation. The calculated equilibrium constant for the formation of free ions have been taken as a quantitative measure of the base strength in IL solutions and compared with the relative constants in water. The effect of IL composition has been discussed for a series of fixed IL anion and fixed IL cation. Finally, the sensitivity of the proton transfer reaction to the electronic effect of the substituent groups on the pyridine ring has been quantified by applying the Hammett equation. A more marked levelling effect on the base strength was observed in ILs than in water. The Hammett reaction constants, rho, were then correlated with some solvent parameters, according to a multiparametric analysis which shows that both specific hydrogen bond donor/acceptor and non-specific interactions play an important role, with alpha and permittivity being the main parameters affecting the IL ability to differentiate the strength of the base.

    更新日期:2017-12-13
  • ChemPlusChem Champions Early Career Researchers
    ChemPlusChem (IF 2.797) Pub Date : 2017-12-13
    Marisa Spiniello
    更新日期:2017-12-13
  • Tuning the Color Temperature of White-Light-Emitting Electrochemical Cells by Laser-Scanning Perovskite-Nanocrystal Color Conversion Layers
    ChemPlusChem (IF 2.797) Pub Date : 2017-12-12
    Wen-Kuang Wu, Cheng-Ming Wang, Ming-Che Chan, Jiun-Yi Lien, Yong-Ming Su, Monima Sarma, Zu-Po Yang, Hai-Ching Su, Ken-Tsung Wong, Sue-Lein Wang
    更新日期:2017-12-12
  • Strategies toward long-life light-emitting electrochemical cells
    ChemPlusChem (IF 2.797) Pub Date : 2017-12-11
    Jun Gao

    This mini-review examines the operational lifetime of light-emitting electrochemical cells (LECs). Under continuous operation, both polymer-based LECs (PLECs) and ionic transition metal complex (iTMC)-based LECs (iTMC-LECs) now exhibit a luminance half-life exceeding 1,000 hours. This improved performance is accomplished with several effective strategies aimed at optimizing the operating scheme, the material composition, and the device architecture. These strategies are presented in detail with PLECs as an example. iTMC-LECs are also highlighted due to their excellent stress stability with regards to both luminance and operating voltage. The survey of literature data points to clear trends, as well as some unexpected results in LECs stressed for an extended period. Major challenges still exist, but long-lasting LECs are possible when the proven strategies are combined with innovative materials and device design.

    更新日期:2017-12-12
  • Trifluoroethoxy-coated Subphthalocyanines Attract Small Arenes in their π-Concave Cavity
    ChemPlusChem (IF 2.797) Pub Date : 2017-12-09
    Satoru Mori, Jiandong Wang, Etsuko Tokunaga, Motoo Shiro, Takashi Matsumoto, Seiji Tsuzuki, Norio Shibata

    X-ray crystallographic analyses of a series of trifluoroethoxy-coated subphthalocyanines disclosed that a molecule of toluene is clasped within the center of the molecular concave cavity. Twelve trifluoroethoxy substitutions, which flexibly surround the toluene molecule to hold it in a 14π-electron conjugated space of subphthalocyanines, can also catch a molecule of benzene. On the other hand, a single non-substituted subphthalocyanine does not show the same phenomena, while two are be required to maintain a small aromatic compound in their cavity after incorporation. DFT calculations of the complexes were attempted to understand the arene clathrates. We believe that there is potential in using trifluoroethoxy-coated subphthalocyanines to prepare arene clathrates as a result of their concave space which is a unique tool to reveal X-ray crystallographic structures of small aromatic molecules of non-crystal, liquid character.

    更新日期:2017-12-11
  • Synthesis of Nontoxic Protoflavone Derivatives through Selective Continuous-Flow Hydrogenation of the Flavonoid B-Ring
    ChemPlusChem (IF 2.797) Pub Date : 2017-12-07
    Sándor B. Ötvös, Máté Vágvölgyi, Gábor Girst, Ching-Ying Kuo, Hui-Chun Wang, Ferenc Fülöp, Attila Hunyadi
    更新日期:2017-12-07
  • Optical Techniques for Light-Emitting Electrochemical Cells
    ChemPlusChem (IF 2.797) Pub Date : 2017-12-05
    Hai-Ching Su

    The concept of solid-state light-emitting electrochemical cells (LECs) proposed in 1995 opened a new field in display and lighting technologies. The key advantage of this technology is based on a single emissive layer containing an emissive material and an ionic salt. Mobile ions in the emissive layer induce electrochemical doping at electrodes and thus the operation voltage can be reduced even by using air-stable electrodes. Since the first demonstration of LECs, many material-oriented efforts have been made in improving device performance of LECs. However, some difficulties arising from material properties still limit further optimizing device characteristics of LECs. Recently, optical techniques have been shown to achieve better device properties without employing new materials. Light extraction techniques recycle the light trapped in layered device structure and thus enhance device light output and efficiency of LECs. Recombination zone probing technique offers direct evidence of carrier balance in LECs and is helpful in optimizing device performance. Spectral filtering based on microcavity effect and localized surface plasmon resonance from metal nanoparticles show advantages of easy fabrication and compatibility with device processing of LECs. This minireview provides a brief overview of the three categories in recent advances of optical techniques of LECs.

    更新日期:2017-12-06
  • Electrodeposited Poly(thieno[3,2-b]thiophene) Films for the Templateless Formation of Porous Structures by Galvanostatic and Pulse Deposition
    ChemPlusChem (IF 2.797) Pub Date : 2017-12-06
    Gabriela Ramos Chagas, Raziyeh Akbari, Guilhem Godeau, Mohammadreza Mohammadizadeh, Frédéric Guittard, Thierry Darmanin
    更新日期:2017-12-06
  • Spectroscopic Engineering toward Near-Infrared Absorption of Materials Containing Perylene Diimide
    ChemPlusChem (IF 2.797) Pub Date : 2017-12-06
    Jonathan R. Cann, Clement Cabanetos, Gregory C. Welch
    更新日期:2017-12-06
  • Linear and Third-Order Nonlinear Optical Properties of Triazobenzene-1,3,5-triazinane-2,4,6-trione (Isocyanurate) Derivatives
    ChemPlusChem (IF 2.797) Pub Date : 2017-12-04
    Ziemowit Pokladek, Marta Dudek, Olivier Mongin, Rémi Métivier, Piotr Mlynarz, Marek Samoc, Katarzyna Matczyszyn, Frédéric Paul
    更新日期:2017-12-04
  • Linear and Third-Order Nonlinear Optical Properties of Triazobenzene-1,3,5-triazinane-2,4,6-trione (Isocyanurate) Derivatives
    ChemPlusChem (IF 2.797) Pub Date : 2017-12-04
    Ziemowit Pokladek, Marta Dudek, Olivier Mongin, Rémi Métivier, Piotr Mlynarz, Marek Samoc, Katarzyna Matczyszyn, Frédéric Paul
    更新日期:2017-12-04
  • The Effect of the Dielectric Constant and Ion Mobility in Light Emitting Electrochemical Cells
    ChemPlusChem (IF 2.797) Pub Date : 2017-11-29
    Lyndon Bastatas, Matthew D. Moore, Jason D. Slinker

    Light emitting electrochemical cells (LEECs) are a promising low-cost option for display and solid state lighting. In these devices, interplay of mobile ions, electrons, and holes makes for rich physics that can be leveraged for high performance. One example of this interplay is in the formation and radiative decay of excitons—bound electron and hole pairs. Considerations from exciton binding and Langevin recombination suggest that a low dielectric constant (ε) would enhance emission. However, emission is also enhanced by the product of the bulk hole and electron concentrations, which in LEECs are enhanced by small mobile ions yielding high dielectric constants. These competing effects make it difficult to predict whether active layers with low or high dielectric constants will optimize device performance. Here, we studied the effect of varying the dielectric constant on the performance of LEEC devices from ionic transition metal complexes by systematically exchanging the negative counterions paired with an iridium complex emitter. We performed electrochemical impedance spectroscopy, constant voltage and constant current device studies, and drift-diffusion simulations. Our results clarify the competing effects of Langevin bimolecular recombination and ion-assisted injection processes occurring in LEECs.

    更新日期:2017-11-30
  • Synthetic Access to Pure Polyradical Architecture: Nucleophilic Insertion of Nitronyl Nitroxide on Cyclotriphosphazene Scaffold
    ChemPlusChem (IF 2.797) Pub Date : 2017-11-29
    catherine Hirel, Ismail Fidan, Emel Önal, Yusuf Yerli, Dominique Luneau, Vefa Ahsen

    An optimized nucleophilic synthetic approach based on mild oxidant and microwave energy was utilized to circumvent the classical Ullman procedure and access poly-nitronyl nitroxide radical easily and in pure form. The simultaneously controlled introduction of preformed nitronyl nitroxide radical on cyclotriphosphazene core allows to obtain a novel polyphosphazene monomers suitable for both n- and p-type redox-active material in organic rechargeable batteries as demonstrated by electrochemistry. Additionally, absorption spectra and Square-Wave Voltammetry were utilized to quantify the number of nitronyl nitroxide radical units on cyclotriphosphazene scaffold.

    更新日期:2017-11-29
  • Three-Dimensional Network Structures Based on Pyridyl-Calix[4]Arene Metal Complexes
    ChemPlusChem (IF 2.797) Pub Date : 2017-11-29
    Carmelo Sgarlata, Giovanna Brancatelli, Cosimo G. Fortuna, Domenico Sciotto, Silvano Geremia, Carmela Bonaccorso
    更新日期:2017-11-29
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  • Triptycene-Bisaroyleneimidazoles as Non-Fullerene Acceptors- The Missing Links
    ChemPlusChem (IF 2.797) Pub Date : 2017-11-23
    Michael Mastalerz, Elisabeth Menke, Felix Berger, Yana Vaynzof, David Leibold, Frank Rominger

    The syntheses of four triptycene-diaroyleneimidazoles - the missing links with respect to the previously reported triptycene-monoaroyleneimidazoles and triptycene-trisaroyleneimidazoles - are presented. Their optoelectronic properties and their use as non-fullerene acceptors in organic photovoltaics (OPVs) with PTB7 as donor are described, reaching a maximum power conversion efficiency of 2%. Furthermore, the effect of molecular symmetry on the photovoltaic device performance is discussed.

    更新日期:2017-11-23
  • Influence of the Anion on the Oxidation of 5-Hydroxymethylfurfural by Using Ionic-Polymer-Supported Platinum Nanoparticle Catalysts
    ChemPlusChem (IF 2.797) Pub Date : 2017-11-22
    Sviatlana Siankevich, Simone Mozzettini, Felix Bobbink, Shipeng Ding, Zhaofu Fei, Ning Yan, Paul J. Dyson
    更新日期:2017-11-22
  • Influence of the Anion on the Oxidation of 5-Hydroxymethylfurfural by Using Ionic-Polymer-Supported Platinum Nanoparticle Catalysts
    ChemPlusChem (IF 2.797) Pub Date : 2017-11-22
    Sviatlana Siankevich, Simone Mozzettini, Felix Bobbink, Shipeng Ding, Zhaofu Fei, Ning Yan, Paul J. Dyson
    更新日期:2017-11-22
  • Peripheral substitution of tetraphenyl porphyrins: Fine-tuning of the self-assembling towards enhanced electroluminescence
    ChemPlusChem (IF 2.797) Pub Date : 2017-11-18
    Athanassios Georgios Coutsolelos, Asterios Charisiadis, Anthi Bagaki, Elisa Fresta, Katharina T. Weber, Georgios Charalambidis, Christina Stangel, Antonios G. Hatzidimitriou, Panagiotis A. Angaridis, Rubén D. Costa

    In this study, we report the preparation of two novel zinc-porphyrin families (ZnTEPP, ZnTHPP and ZnTDPP as well as ZnTbEPP, ZnTbHPP and ZnTbDPP) bearing four or eight alkoxy chains at their peripheral phenyl rings, respectively. The length of the alkyl-chains varies from 2, to 6 and to 12 carbon atoms. All the modified zinc-porphyrin derivatives were fully characterized with respect to their photophysical and electrochemical features. Upon changing the length of the aryl peripheral substitution, we were able to fabricate thin-films with ordered and disordered nature as determined using spectroscopic and miscroscopic techniques. The films containing ordered self-assemblies led to a significantly enhanced electrical conductivity compared to that of the disordered films. This led to remarkable differences regarding the electroluminescence response that occurs at lower bias with a luminous efficiency of almost one order of magnitude higher when comparing ordered with disordered films.

    更新日期:2017-11-19
  • Polyradical PROXYL/TEMPO-Derived Amides: Synthesis, Physicochemical Studies, DFT Calculations, and Antimicrobial Activity
    ChemPlusChem (IF 2.797) Pub Date : 2017-11-17
    Patrik Poprac, Peter Poliak, Miroslav Kavala, Zuzana Barbieriková, Michal Zalibera, Marek Fronc, Ľubomír Švorc, Zuzana Vihonská, Petra Olejníková, Karol Lušpai, Vladimír Lukeš, Vlasta Brezová, Peter Szolcsányi
    更新日期:2017-11-17
  • A Two-Photon Luminescent Dye-Loaded Metal–Organic Framework for Physiological Temperature Sensing within Biological Windows
    ChemPlusChem (IF 2.797) Pub Date : 2017-11-15
    Yating Wan, Tifeng Xia, Yuanjing Cui, Yu Yang, Guodong Qian
    更新日期:2017-11-16
  • Anchoring a Sulfonate Group to an Electron-transporting Molecule via an Alkyl Chain and Its Use as the Counter-anion in a Phosphorescent Cationic Iridium Complex
    ChemPlusChem (IF 2.797) Pub Date : 2017-11-15
    Lei He, Pei Wang, Ningzi Luo, xiangzhi Song

    We report an electron-transporting anion prepared by anchoring a sulfonate group onto an electron-transporting molecule via a flexible alkyl chain and its use as the counter-anion in a cationic iridium complex. The flexible alkyl chain improves the solubility of the bulky anion in water or in polar organic solvent. The anion exhibits similar photophysical and electrochemical properties to the parent electron-transporting molecule. Within the complex, the anion does not disturb the the phosphorescence of the cation in the solid film. Solution-processed small-molecule organic light-emitting diodes (OLEDs) using the complex as the dopant show superior performances over the reference device using the conventional complex with a PF6− counter-anion. It is revealed that anchoring anionic groups to optoelectronically active molecules via flexible alkyl chains is a feasible approach to develop optoelectronically active anions for assembling ion pairs with advanced optoelectronic properties.

    更新日期:2017-11-15
  • Electronic structure calculations and experimental studies on the thermal initiation of the twin polymerization process
    ChemPlusChem (IF 2.797) Pub Date : 2017-11-15
    Alexander A Auer, Giovanni Bistoni, Philipp Kitschke, Michael Mehring, Thomas Ebert, Stefan Spange

    We present a combined computational and experimental study on the thermal initiation process of the twin polymerization. While the thermally initiated twin polymerization offers a versatile scheme for obtaining hybrid organic/inorganic nanocomposite materials, the mechanism for its initiation is very different from the proton initiated twin polymerization. We investigate the basic mechanism of the early steps of the polymerization process of 4H,4H'-2,2'-spirobi[benzo[d][1,3,2]dioxasiline] using electronic structure calculations in conjunction with experimental differential scanning calorimetry studies. This way, the influences on the thermally initiated twin polymerization process can be analyzed in detail. We systematically assess previous mechanistic hypotheses and show that based on our results, a new hypothesis for an initiation mechanism can be formulated that is in agreement with all experimental observations. Our results suggest that, before the formation of the polymer networks, the thermal initiation starts with the formation of low-molecular weight fragments that react to yield acidic groups. If a sufficient amount of these have been formed, the reaction is ultimately funneled into a mechanism similar to the one of the proton initiated twin polymerization.

    更新日期:2017-11-15
  • Photoinitiating Systems Based on Anthraquinone Derivatives: Synthesis of Antifouling and Biocide Coatings
    ChemPlusChem (IF 2.797) Pub Date : 2017-11-09
    Somia Tomane, Pauline Sautrot-Ba, Pierre-Emmanuel Mazeran, Jacques Lalevée, Bernadette Graff, Fabrice Morlet-Savary, Samir Abbad-Andaloussi, Valérie Langlois, Davy-Louis Versace
    更新日期:2017-11-09
  • 更新日期:2017-11-08
  • A two-photon luminescent dye-loaded MOF for physiological temperature sensing working within biological windows
    ChemPlusChem (IF 2.797) Pub Date : 2017-11-06
    Yating Wan, Tifeng Xia, Yuanjing Cui, Yu Yang, Guodong Qian

    Luminescent temperature sensing in biological windows has unique superiority compared to traditional temperature sensing methods for the scattering and absorption by skin, tissue and blood is minimum. Here, for the first time we utilized two-photon luminescence from dyes loaded in framework of metal-organic framework (MOF) and realized physiological temperature sensing within two biological windows. The composite ZJU-28DPASD was prepared and can be excited by 1064 nm while emits at 650 nm exactly locating at the two biological windows. The two-photon luminescent intensity at 650 nm has a linear relationship with temperature in a range from 20 oC to 60 oC. In addition, the stability and quantum efficiency were significantly improved after loading, with high temperature resolution, excellent repeatability and reduced biological toxicity, the composite has great potential to be applied for physiological temperature sensing in cell or tissue.

    更新日期:2017-11-06
  • Solvent, Cation and Anion Induced Structure Variations in Manganese-based TCNQF4 Complexes: Synthesis, Crystal Structures, Electrochemistry and their catalytic properties
    ChemPlusChem (IF 2.797) Pub Date : 2017-11-02
    Jinzhen Lu, Brendan Abrahams, Robert Elliott, Richard Robson, Alan Bond, Lisandra Martin

    The reaction of Mn(BF4)2∙xH2O with (Pr4N)2TCNQF4 in a mixture of methanol/dichloromethane (CH3OH/CH2Cl2) gives a 2:3 stoichiometric complex of (Pr4N)2[Mn2(TCNQF4)3(CH3OH)2] (1). If the solvent system used for crystallisation of 1 is changed to methanol/dimethylformamide (CH3OH/DMF), then a different product [Mn(TCNQF4)(DMF)2]∙(CH3OH)2 (2) is obtained. The use of Li2TCNQF4 instead of (Pr4N)2TCNQF4 leads to the generation of [Mn2(TCNQF4)2(DMF)4]∙3(DMF) (3). An unexpected mixed oxidation state network with a composition [MnII4MnIII16O10(OH)6(OCH3)24(TCNQF4)2(NO3)2·24(CH3OH) (4), is formed if Mn(NO3)2∙xH2O is used in place of Mn(BF4)2∙xH2O in the reaction that leads to the formation of 3. Compounds 1, 2 and 3 have been characterised by X-ray crystallography, FTIR, Raman, UV/vis spectroscopy and electrochemistry. Compound 4 has been analysed only by X-ray crystallography and vibrational spectroscopy (Raman, FTIR) due to rapid deterioration of the compound upon exposure to the atmosphere. These results indicate that relatively minor changes in reaction conditions have the potential to yield products with vastly different structures. Compound 1 adopts a novel anionic 2D network with unusual π-stacked dimers of the TCNQF42- dianion, whereas 2 and 3 are composed of similar neutral sheets of [Mn(TCNQF4)(DMF)2].

    更新日期:2017-11-03
  • 更新日期:2017-11-03
  • Mesoporous Copper Nanoparticle Networks Decorated by Graphite Layers for Surface-Enhanced Raman Scattering Detection of Trace Analytes
    ChemPlusChem (IF 2.797) Pub Date : 2017-10-26
    Georgia Velegraki, Jian Xie, Qichun Zhang, Gerasimos S. Armatas
    更新日期:2017-10-27
  • A Ferrocene–Tryptophan Conjugate: The Role of the Indolic Nitrogen in Supramolecular Assembly
    ChemPlusChem (IF 2.797) Pub Date : 2017-10-24
    Natashya Falcone, Shibaji Basak, Bin Dong, Jebriel Syed, Annaleizle Ferranco, Alan Lough, Zhe She, Heinz-Bernhard Kraatz
    更新日期:2017-10-24
  • Polyradical PROXYL/TEMPO-derived Amides: Synthesis, Physicochemical Studies, DFT Calculations, and Antimicrobial Activity
    ChemPlusChem (IF 2.797) Pub Date : 2017-10-20
    Patrik Poprac, Peter Poliak, Miroslav Kavala, Zuzana Barbieriková, Michal Zalibera, Marek Fronc, Ľubomír Švorc, Zuzana Vihonská, Petra Olejníková, Karol Lušpai, Vladimír Lukeš, Vlasta Brezová, Peter Szolcsányi

    A series of polynitroxide amides possessing PROXYL and/or TEMPO units connected with various bridges were synthesized and their properties were analyzed using multiple experimental techniques. EPR spectroscopy provided a detailed insight into their paramagnetic character and related properties. The thorough examination of EPR spectra of dinitroxides in organic solvents brought valuable information on the intramolecular motions, thermodynamics and spin exchange mechanisms. The analysis of low-temperature X- and Q-band EPR spectra of the dissolved dinitroxides provided the spin-spin distances comparable with the theoretical values evaluated by DFT. Cyclic voltammetry investigations revealed (quasi)reversible electrochemical behaviour for PROXYL-derived biradicals, while significant loss of the reversibility was found for TEMPO-containing biradicals and polyradicals. The assessment of inhibitory activities of studied nitroxides against model bacteria, yeasts and filamentous fungi was conducted. Generally, the best inhibition was observed in the case of S. epidermidis, while the most active TEMPO containing tetra- and hexaradical also inhibited the growth of S. aureus. A rather weak growth inhibition of yeast and/or filamentous fungi was obtained for most of the tested nitroxides, revealing again the highest antifungal activity for the polynitroxides. Significantly, no mutagenic properties of tetra- and hexanitroxides with highest antibacterial activity was found.

    更新日期:2017-10-20
  • Influence of the Anion on the Oxidation of 5-Hydroxymethylfurfural by Using Ionic-Polymer-Supported Platinum Nanoparticle Catalysts
    ChemPlusChem (IF 2.797) Pub Date : 2017-10-20
    Sviatlana Siankevich, Simone Mozzettini, Felix Bobbink, Shipeng Ding, Zhaofu Fei, Ning Yan, Paul J. Dyson
    更新日期:2017-10-20
  • Vacuum-deposited versus spin-coated emissive layers toward fabricating high-performance blue-green-emitting diodes
    ChemPlusChem (IF 2.797) Pub Date : 2017-10-19
    Lian Duan, Dongxin Ma, Yong Qiu

    We investigated and discussed the electroluminescent characteristics of two sublimable cationic iridium(III) complexes bearing the same coordinated iridium(III) cation while different tetraphenylborate-type negative counter-ions. Blue-green-emitting devices thereof were successfully fabricated using various preparation processes, spin-coating and vacuum evaporation deposition, respectively. Experiments indicated that compared to devices with spin-coated emissive layers, the ones with vacuum-deposited layers showed superior photo-electric properties including a maximum current efficiency of 27.91 cd/A, external quantum efficiency of 10.48 %, power efficiency of 27.73 lm/W and highest luminance up to 25.34×103 cd/m2, while the turn-on voltages were quite low. The overall device performance has surely ranked among best results of phosphorescent organic light-emitting diodes based on ionic transition metal complexes.

    更新日期:2017-10-19
  • 更新日期:2017-10-19
  • Pd-Complexes of Carbazole-Based Chalcogenaisophlorins: Synthesis, Structure, and Solid-State NIR Absorption
    ChemPlusChem (IF 2.797) Pub Date : 2017-10-17
    Chihiro Maeda, Kazuto Takaishi, Tadashi Ema

    Annulation reactions of butadiyne-bridged carbazole dimer 1 produced carbazole-based chalcogenaisophlorins 2-4 which were transformed into the corresponding Pd-complexes 2Pd-4Pd. The structures were characterized by NMR spectroscopy and X-ray diffraction analysis. Metallation fixed the structures to generate small antiaromatic character derived from 20π-isophlorin. They showed weak near infrared (NIR) absorption typical for antiaromatic porphyrinoids in solution. In addition, 2Pd and 3Pd showed relatively strong solid-state NIR absorption. X-ray diffraction analyses of 2Pd and 3Pd revealed trimeric and dimeric stacked-layered structures, respectively, and DFT calculations suggest that the solid-state NIR absorption is ascribed to intermolecular charge transfer.

    更新日期:2017-10-17
  • Real-Time Reaction Monitoring of an Organic Multistep Reaction by Electrospray Ionization-Ion Mobility Spectrometry
    ChemPlusChem (IF 2.797) Pub Date : 2017-10-13
    Martin Zühlke, Stephan Sass, Daniel Riebe, Toralf Beitz, Hans-Gerd Löhmannsröben
    更新日期:2017-10-13
  • Mesoporous Cu Nanoparticle Networks Decorated by Graphite Layers for Surface-Enhanced Raman Scattering Detection of Trace Analytes
    ChemPlusChem (IF 2.797) Pub Date : 2017-10-10
    Georgia Velegraki, Jian Xie, Qichun Zhang, Gerasimos S. Armatas

    Assembling 3D nanoscale structures of plasmonic nanoparticles (NPs) holds great promise for achieving enhanced optical and electronic properties. This type of materials exhibits a large number of surface hot spots, while offer the possibility for synergetic effects to be observed. In this study, we demonstrate a facile, yet powerful, strategy to fabricate 3D mesoporous networks of Cu NPs decorated with graphite layers (denoted as Cu/G) using a polymer-assisted self-assembly method. We show that, after thermal processing, the resulting Cu/G NP-linked networks retain an open and interconnected porosity with large surface area (up to 90 m2 g-1) and narrow pore-size distribution (ca. 4.3 nm in size). Owing to these characteristics, Cu/G assemblies behave as high-performance surface-enhanced Raman scattering (SERS) probes for the detection of analytes in very low concentrations. The substrates comprise low-cost, environmental benign materials and show promise for chemical and biological sensing applications.

    更新日期:2017-10-10
  • Photoinitiating Systems based on Anthraquinone Derivative: a Key Role in the Synthesis of Antifouling and Biocide Coatings upon Light Exposure
    ChemPlusChem (IF 2.797) Pub Date : 2017-10-10
    Davy-Louis Versace, Somia Tomane, Pauline Sautrot-Ba, Pierre-Emmanuel Mazeran, Valerie Langlois, Jacques Lalevee, Samir Abbad-Andaloussi, Fabrice Morlet-Savary, Bernadette Graff

    Performing photoinitiating systems combining 2, 6-Diaminoanthraquinone (AQD), iodonium salt (Iod) and benzyl alcohol derivatives have been developed to efficiently initiate the cationic polymerization of epoxy monomer upon light exposure. Electron Spin Resonance spin-trapping (ESR ST) experiments, fluorescence investigations and steady state photolysis have demonstrated that a dye-sensitized reaction occurs between AQD and the benzyl alcohol derivatives via a H-abstraction mechanism upon light illumination, followed by a reduction of Iod. The in situ liberation of protic acids promotes the cationic photopolymerization of epoxy monomers concomitantly with hydrolysis and condensation of the reactive methoxysilanes of an organic-inorganic precursor e.g. 3-Glycidyloxypropyltrimethoxysilane (GPTMS). Nanoindentation experiments and scratch resistance tests proved that the resulting GPTMS coatings exhibit very good resistance to brittle fracture and excellent adherence to the stainless steel substrates. Interestingly, the antibacterial tests on the GPTMS coatings have highlithed efficient antifouling and biocide properties against E. coli and S. aureus.

    更新日期:2017-10-10
  • Amperometric Detection of dsDNA using an Acridine-Orange-Modified Glucose Oxidase
    ChemPlusChem (IF 2.797) Pub Date : 2017-10-10
    Daliborka Jambrec, Klaus Lammers, Tim Bobrowski, Sascha Pöller, Wolfgang Schuhmann, Adrian Ruff
    更新日期:2017-10-10
  • Assembly of Nitrofurazan and Nitrofuroxan Frameworks for High-Performance Energetic Materials
    ChemPlusChem (IF 2.797) Pub Date : 2017-10-10
    Leonid L. Fershtat, Igor V. Ovchinnikov, Margarita A. Epishina, Anna A. Romanova, David B. Lempert, Nikita V. Muravyev, Nina N. Makhova
    更新日期:2017-10-10
  • Catalysis and CO2 Capture by Palladium-Incorporated Covalent Organic Frameworks
    ChemPlusChem (IF 2.797) Pub Date : 2017-10-09
    Dhananjayan Kaleeswaran, Rajendran Antony, Abhishek Sharma, Ateeque Malani, Ramaswamy Murugavel
    更新日期:2017-10-09
  • Influence of the anion on the oxidation of 5-hydroxymethylfurfural using platinum nanoparticle-ionic polymer supported catalysts.
    ChemPlusChem (IF 2.797) Pub Date : 2017-10-03
    Sviatlana Siankevich, Simone Mozzettini, Felix Daniel Bobbink, Shipeng Ding, Zhaofu Fei, Ning Yan, Paul J. Dyson

    Platinum nanoparticles coated with an imidazolium-based cross-linked polymer (with chloride as the counter anion) efficiently catalyze the oxidation of 5-hydroxymethylfurfural to 2,5-furandicarboxylic acid in water under mild conditions using oxygen as the oxidant. In this paper we explore this catalyst system by varying the counter anion, i.e. replacing chloride by BF4-, PF6-, bis(trifluoromethylsulfonyl)imide, hexanoate or laurate anions, in the cationic polymer. The counter-anion influences both the structure of the obtained platinum nanoparticles, the surface electronic properties and their catalytic activity. Highest reaction rates were obtained with the weakly-nucleophilic bis(trifluoromethylsulfonyl)imide anion, which also favors platinum in the zero oxidation state, leading to complete conversion of the substrate and a high yield of 2,5-furandicarboxylic acid under mild conditions.

    更新日期:2017-10-03
  • Ferrocene-Tryptophan Conjugate: Role of Indolic Nitrogen In Supramolecular Assembly
    ChemPlusChem (IF 2.797) Pub Date : 2017-10-02
    Natashya Falcone, Shibaji Basak, Bin Dong, Jebreil Syed, Annaleizle Ferranco, Alan Lough, Zhe She, Heinz-Bernhard Kraatz

    The synthesis of supramolecular gels has attracted a lot of attention due to their wide range of applications in drug delivery, biomimics, environmental studies, and materials science. Bio-organometallic ferrocene amino acids and peptides have been reported to form gels and are interesting to study due to their structural properties and applications for biological purposes. In this research a ferrocene dicarboxylic acid derivative of the dipeptide, tryptophan-tryptophan was explored. The indolic nitrogen in the amino acid tryptophan is significant in biological functions due to its role in hydrogen bonding. Here, intermolecular interactions with the indolic nitrogen allow this conjugate to self-assemble into a fibrous supramolecular structure which forms a stable gel. Rheological analysis demonstrates the self-healing nature of this gel. Interestingly, X-ray analysis of compound 1 highlights close contacts involving Trp, involving the indole NH in interactions with an adjacent neighbouring molecule.

    更新日期:2017-10-03
  • Site-Selective Labeling of Chromium(III) as a Quencher on DNA for Molecular Beacons
    ChemPlusChem (IF 2.797) Pub Date : 2017-10-02
    Huan Ma, Wang Li, Wenhu Zhou, Juewen Liu
    更新日期:2017-10-03
Some contents have been Reproduced with permission of the American Chemical Society.
Some contents have been Reproduced by permission of The Royal Society of Chemistry.
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