ChemPhysChem

Cover image for Vol. 10 Issue 7

May 11, 2009

Volume 10, Issue 7

Pages 989–1147

  1. Cover Picture

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    1. Cover Picture: Local Modulation of the Redox State of p-Nitrothiophenol Self-Assembled Monolayers Using the Direct Mode of Scanning Electrochemical Microscopy (ChemPhysChem 7/2009) (page 989)

      Stefanie Schwamborn, Leonard Stoica, Sebastian Neugebauer, Torsten Reda, Hanns-Ludwig Schmidt and Wolfgang Schuhmann

      Article first published online: 4 MAY 2009 | DOI: 10.1002/cphc.200990026

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      The cover picture illustrates the principle of molecular writing using direct-mode scanning electrochemical microscopy (SECM). The redox state of the end groups of a p-nitrothiophenol self-assembled monolayer (SAM) is selectively reduced either to the hydroxylamine/nitoso redox couple or to the amino group. Besides the writing procedure, W. Schuhmann et al. demonstrate on p. 1066 that SECM can also be utilized for visualization or reading of the generated microstructure in feedback mode using hexacyanoferrate as redox mediator.

  2. Graphical Abstract

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    1. Graphical Abstract: ChemPhysChem 7/2009 (pages 991–998)

      Article first published online: 4 MAY 2009 | DOI: 10.1002/cphc.200990027

  3. News

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  4. Minireview

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    1. Tailoring Disorder and Dimensionality: Strategies for Improved Solid Oxide Fuel Cell Electrolytes (pages 1003–1011)

      Javier Garcia-Barriocanal, Alberto Rivera-Calzada, Maria Varela, Zouhair Sefrioui, Mario R. Díaz-Guillén, Karla J. Moreno, José A. Díaz-Guillén, Enrique Iborra, Antonio F. Fuentes, Stephen J. Pennycook, Carlos Leon and Jacobo Santamaria

      Article first published online: 27 MAR 2009 | DOI: 10.1002/cphc.200800691

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      Towards cooler solid oxide fuel cells: Disorder and dimensionality (see picture) play an important role in determining ion mobility of bulk and artificially nanolayered materials and should be considered in the design of new electrolytes with enhanced conductivity.

  5. Communications

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    1. Reversible Structural Modulation of Fe–Pt Bimetallic Surfaces and Its Effect on Reactivity (pages 1013–1016)

      Teng Ma, Qiang Fu, Hai-Yan Su, Hong-Yang Liu, Yi Cui, Zhen Wang, Ren-Tao Mu, Wei-Xue Li and Xin-He Bao

      Article first published online: 27 APR 2009 | DOI: 10.1002/cphc.200900053

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      Tunable surface: The surface structure of the Fe–Pt bimetallic catalyst can be reversibly modulated between the iron-oxide-rich Pt surface and the Pt-skin structure with subsurface Fe via alternating reduction and oxidation treatments (see figure). The regenerated active Pt-skin structure is active in reactions involving CO and/or O.

    2. In Situ Plasmon-Heating-Induced Generation of Au/TiO2 “Hot Spots” on Colloidal Crystals (pages 1017–1022)

      Ivano Alessandri, Matteo Ferroni and Laura E. Depero

      Article first published online: 23 MAR 2009 | DOI: 10.1002/cphc.200900080

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      SERS you right: The plasmon heating of gold nanoshells is exploited to yield the local conversion of amorphous TiO2 into anatase on the surface of polymeric colloidal crystals (see scheme). The resulting Au/TiO2 spots are active substrates for surface-enhanced Raman spectroscopy and allow surface reactions and processes to be followed directly on-site.

    3. Exciton Binding Energies in Conjugated Polyelectrolyte Films (pages 1023–1027)

      Jung Hwa Seo, Youngeup Jin, Jacek Z. Brzezinski, Bright Walker and Thuc-Quyen Nguyen

      Article first published online: 19 FEB 2009 | DOI: 10.1002/cphc.200800751

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      Molecular design: The electronic structure of conjugated polyelectrolytes as a function of ionization potential (IP) and electron affinity (EA) is determined using X-ray absorption and emission spectroscopy (see figure). Different functional groups give rise to dissimilar transport gaps and exciton binding energies.

    4. Size Dependence of Molar Absorption Coefficients of CdSe Semiconductor Quantum Rods (pages 1028–1031)

      Ehud Shaviv, Asaf Salant and Uri Banin

      Article first published online: 3 APR 2009 | DOI: 10.1002/cphc.200800874

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      Fundamental properties: The molar absorption coefficients of CdSe quantum rods are determined experimentally as a function of their dimensions (see figure). Far above the band gap a simple dependence on volume is seen. The behavior at the band gap manifests a concentration of oscillator strength with decreased diameter in agreement with strong quantum confinement behavior.

    5. Robust Supramolecular Network on Ag(111): Hydrogen-Bond Enhancement through Partial Alcohol Dehydrogenation (pages 1032–1035)

      Remy Pawlak, Sylvain Clair, Vincent Oison, Mathieu Abel, Oualid Ourdjini, Nikolas A. A. Zwaneveld, Didier Gigmes, Denis Bertin, Laurent Nony and Louis Porte

      Article first published online: 30 MAR 2009 | DOI: 10.1002/cphc.200900055

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      Alcohol oxidation and self-assembly: the in situ oxidation of hydroxyl functional groups to quinone groups promotes the formation of enhanced hydrogen bonds and allows reorganization of the resulting supramolecular self-assemblies, which evolve from a weakly bound dense phase to a strongly bound nanoporous open structure (see picture).

  6. Articles

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    1. Redox Properties of Mixed Lutetium/Yttrium Nitride Clusterfullerenes: Endohedral LuxY3−xN@C80(I) (x=0–3) Compounds (pages 1037–1043)

      Ján Tarábek, Shangfeng Yang and Lothar Dunsch

      Article first published online: 9 APR 2009 | DOI: 10.1002/cphc.200800811

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      The complex redox behavior of mixed lutetium/yttrium nitride clusterfullerenes of the series LuxY3−xN§C80(Ih, x=0–3) (see figure) results in up to three irreversible reduction steps. A reduction mechanism is proposed based on fast-scan and square-wave voltammetry experiments combined with simulations of the voltammograms.

    2. Characterizing Pt-Derived Anticancer Drugs from First Principles: The Case of Oxaliplatin in Aqueous Solution (pages 1044–1052)

      Elizabeth C. Beret, Rafael R. Pappalardo, Dominik Marx and Enrique Sánchez Marcos

      Article first published online: 2 MAR 2009 | DOI: 10.1002/cphc.200900027

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      Anionic hydration: Ab initio molecular dynamics simulations help to obtain a microscopic description of the behavior of oxaliplatin anticancer drug in bulk water (see picture). Its hydration structure is closely related to that previously found for PtII aqua ion and derives from the presence of a square-planar motif around the metal center.

    3. Localized Electrografting of Vinylic Monomers on a Conducting Substrate by Means of an Integrated Electrochemical AFM Probe (pages 1053–1057)

      Achraf Ghorbal , Federico Grisotto, Julienne Charlier, Serge Palacin, Cédric Goyer and Christophe Demaille

      Article first published online: 23 MAR 2009 | DOI: 10.1002/cphc.200800803

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      An electrochemical lithographic tool for locally electrografting a non-conducting organic coating on a conducting substrate with a submicrometer resolution is provided by atomic force scanning electrochemical microscopy (AFM-SECM). The picture shows the topographic AFM image of the line pattern drawn with an AFM-SECM tip on a gold surface by direct reduction of an aryl diazonium salt/acrylic acid electrolyte solution.

    4. Computational and Variable-Temperature Infrared Spectroscopic Studies on Carbon Monoxide Adsorption on Zeolite Ca-A (pages 1058–1065)

      Angeles Pulido, Petr Nachtigall, Montserrat Rodríguez Delgado and Carlos Otero Areán

      Article first published online: 13 MAR 2009 | DOI: 10.1002/cphc.200800843

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      Bridged Ca2+⋅⋅⋅CO⋅⋅⋅Ca2+complexes are formed on dual-cation sites, constituted by a pair of nearby Ca2+ cations, when CO is adsorbed on zeolite Ca-A. Two types of such species can be formed, designated S2–S1 and S1–S1 (see picture). Ca2+⋅⋅⋅CO monocarbonyl species are also identified, and at a relatively high CO equilibrium pressure, dicarbonyl complexes can also form.

    5. Local Modulation of the Redox State of p-Nitrothiophenol Self-Assembled Monolayers Using the Direct Mode of Scanning Electrochemical Microscopy (pages 1066–1070)

      Stefanie Schwamborn, Leonard Stoica, Sebastian Neugebauer, Torsten Reda, Hanns-Ludwig Schmidt and Wolfgang Schuhmann

      Article first published online: 25 APR 2009 | DOI: 10.1002/cphc.200900118

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      Local redox conversion of nitro end groups of a 4-nitrothiophenol self-assembled monolayer on gold is achieved by direct-mode scanning electrochemical microscopy (SECM). Potential pulses are applied to the modified gold surface leading to local reduction of nitro end groups to either hydroxylamine (−0.47 V, see picture) or amino groups (−0.6 V) exclusively beneath the positioned SECM tip.

    6. Triplet Excitation Scavenging in Films of Conjugated Polymers (pages 1071–1076)

      Sarah Schols, Andrey Kadashchuk, Paul Heremans, Anke Helfer and Ullrich Scherf

      Article first published online: 16 APR 2009 | DOI: 10.1002/cphc.200900054

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      Nonvertical triplet energy transfer in solid conjugated polymer films is demonstrated for the first time using 1,3,5,7-cyclooctatetraene, a compound that can efficiently quench the phosphorescence of polyfluorene without affecting its fluorescence (see spectra). The results suggest that nonvertical triplet scavengers might be promising candidates for controlling the triplet concentration in fluorescent high-brightness organic devices.

    7. Electron Transfer from Photoexcited TiO2 to Chelating Alizarin Molecules: Reversible Photochromic Effect in Alizarin@TiO2 under UV Irradiation (pages 1077–1083)

      Yesica Di Iorio, Marta A. Brusa, A. Feldhoff and María A. Grela

      Article first published online: 5 MAR 2009 | DOI: 10.1002/cphc.200800752

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      Reduction of alizarin molecules coupled to TiO2 nanoparticles occurs on UV irradiation in the presence of a sacrificial electron donor. Reduction is mediated by conduction-band electrons and yields a 1,2,9,10-tetrahydroxyanthracene species which remains coupled to the TiO2 nanoparticles (see figure). The process can be reversed by addition of an acceptor (i.e. oxygen).

    8. Direct Synthesis of a Photoactive Inorganic–Organic Mesostructured Hybrid Material and its Application as a Photocatalyst (pages 1084–1089)

      Avelino Corma, Maria T. Navarro, Fernando Rey, Violeta R. Ruiz and Maria J. Sabater

      Article first published online: 19 FEB 2009 | DOI: 10.1002/cphc.200800724

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      A direct route: Silylated triphenylmethanol is incorporated into mesoporous material MCM-41 through a direct synthesis method. Under acidic conditions, this inorganic–organic hybrid generates trityl cations to give the photoactive material Tyl-MCM41. Tyl-MCM41 promotes the photosensitized dimerization of 1,3-cyclohexadiene with an unprecedented selectivity towards the formation of the exo product (see scheme).

    9. Photoelectrochemical Studies of Gold Electrodes Chemically Modified with Single-Walled Carbon Nanotubes (pages 1090–1096)

      Daniele Merli, Antonella Profumo, Daniele Dondi and Angelo Albini

      Article first published online: 23 MAR 2009 | DOI: 10.1002/cphc.200800684

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      Seeing the light: An electrode is assembled by linking acid-shortened single-walled carbon nanotubes with carboxylic groups to a gold surface modified with a cysteamine monolayer. The electrode generates a photocurrent when illuminated with visible light in the presence of an electroactive species (see picture). With an appropriate applied potential the device behaves as a photodiode.

    10. Molar Mass, Radius of Gyration and Second Virial Coefficient from new Static Light Scattering Equations for Dilute Solutions: Application to 21 (Macro)molecules (pages 1097–1105)

      Bertrand Illien and Ruifeng Ying

      Article first published online: 23 MAR 2009 | DOI: 10.1002/cphc.200800490

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      New equations for static light scattering of dilute binary solutions allow molar mass determination of macromolecules from measurements of scattered intensity ratios between solution and solvent (Ir). In contrast to the standard Carr–Zimm equations, they do not rely on the experimental absolute value of the Rayleigh ratio of a reference liquid. The picture shows a typical plot for the surfactant BRIJ72 in CH2Cl2 (MSupplier=0.359 kg mol−1).

    11. Multilayer Structures of Self-Assembled Gold Nanoparticles as a Unique SERS and SEIRA Substrate (pages 1106–1111)

      Monica Baia, Felicia Toderas, Lucian Baia, Dana Maniu and Simion Astilean

      Article first published online: 25 MAR 2009 | DOI: 10.1002/cphc.200800815

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      Gold deposits: Multilayer gold nanostructures deposited on a glass substrate are characterized by AFM and UV/Vis spectroscopy. Detailed analysis of the recorded spectra shows the potential of this substrate in surface-enhanced Raman spectroscopy and surface-enhanced IR absorption (see picture) for providing information about the adsorbed species.

    12. Proton Transfer in the Complex H3N⋅⋅⋅HCl Catalyzed by Encapsulation into a C60 Cage (pages 1112–1116)

      Fang Ma, Zhi-Ru Li, Hong-Liang Xu, Zong-Jun Li, Di Wu, Ze-Sheng Li and Feng Long Gu

      Article first published online: 3 APR 2009 | DOI: 10.1002/cphc.200800721

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      Caged up: In contrast to acid–base behavior in solution, single molecules of NH3 and HCl do not react to form the ion pair NH4+Cl in isolation. Proton transfer occurs in the complex H3N⋅⋅⋅HCl inside the C60 cage, to form the ion pair NH4+Cl under the catalytic action of C60 (see picture).

    13. Influence of Sodium Cations of N3 Dye on the Photovoltaic Performance and Stability of Dye-Sensitized Solar Cells (pages 1117–1124)

      Luísa Andrade, Shaik M. Zakeeruddin, Mohammad K. Nazeeruddin, Helena Aguilar Ribeiro, Adélio Mendes and Michael Grätzel

      Article first published online: 23 MAR 2009 | DOI: 10.1002/cphc.200900111

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      Little things count: The number of protons and the nature of cations of the dye influence the open-circuit potential and the short circuit current of dye-sensitized solar cells (DSCs, see picture). Thus, the effect of substituting the two tetrabutylammonium counter ions in the standard N719 dye by sodium ions allows the improvement on the performance and stability of DSCs.

    14. Are Mixed Explicit/Implicit Solvation Models Reliable for Studying Phosphate Hydrolysis? A Comparative Study of Continuum, Explicit and Mixed Solvation Models (pages 1125–1134)

      Shina C. L. Kamerlin, Maciej Haranczyk and Arieh Warshel

      Article first published online: 19 MAR 2009 | DOI: 10.1002/cphc.200800753

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      Are all solvation models equal? An in-depth comparison of mixed implicit/explicit solvation models shows that while both the implicit and explicit (QM/MM–FEP) solvation models can reproduce activation free energies for phosphate diester hydrolysis in solution with high accuracy, the use of a mixed solvation model tends to be unreliable for modelling phosphate hydrolysis in solution.

    15. Photolysis of o-Nitrobenzaldehyde in the Gas Phase: A New OH. Formation Channel (pages 1135–1142)

      Shi-Bo Cheng, Can-Hua Zhou, Hong-Ming Yin, Ju-Long Sun and Ke-Li Han

      Article first published online: 30 MAR 2009 | DOI: 10.1002/cphc.200800735

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      New route to gas-phase OH.: UV photolysis of gaseous o-nitrobenzaldehyde forms OH radicals via the transformation into the ketene or o-nitrosobenzoic acid intermediate (see figure). The OH. product is monitored by single-photon laser-induced fluorescence (LIF).

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      Preview: ChemPhysChem 8/2009 (page 1147)

      Article first published online: 4 MAY 2009 | DOI: 10.1002/cphc.200990025

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