Advanced Materials

Cover image for Vol. 17 Issue 7

April, 2005

Volume 17, Issue 7

Pages 783–934

    1. Cover Picture: Novel Photoactive Single-Walled Carbon Nanotube–Porphyrin Polymer Wraps: Efficient and Long-Lived Intracomplex Charge Separation (Adv. Mater. 7/2005)

      D. M. Guldi, H. Taieb, G. M. A. Rahman, N. Tagmatarchis and M. Prato

      Article first published online: 30 MAR 2005 | DOI: 10.1002/adma.200590036

      Novel donor-acceptor nanoassemblies (see cover) are prepared using pristine single-walled carbon nanotubes (SWNTs) as electron-acceptor components in supramolecular “polymer wraps”, with poly(methyl methacrylate) carrying porphyrin units (H2P) as excited-state electron donors (see Figure). In these novel donor–acceptor ensembles, SWNTs quench the photoexcited H2P chromophores, resulting in the creation of long-lived radical ion pairs.

    2. Contents: Adv. Mater. 7/2005 (pages 783–793)

      Article first published online: 30 MAR 2005 | DOI: 10.1002/adma.200590034

    3. Silicon Nanocrystals: Size Matters (pages 795–803)

      J. Heitmann, F. Müller, M. Zacharias and U. Gösele

      Article first published online: 30 MAR 2005 | DOI: 10.1002/adma.200401126

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      Silicon nanocrystals are candidates for silicon-based light-emitting devices and non-volatile memories—provided that size control can be realized. In recent years, various approaches of narrowing the size distribution of silicon nanocrystals have been developed by introducing new synthetic techniques, such as incorporation into SiO2 matrices to form superlattices (see Figure). The most promising recently developed approaches are reviewed, and their potential for silicon-nanocrystal applications is discussed.

    4. Control of Nanometer-Scale Tunnel Sizes of Porous Manganese Oxide Octahedral Molecular Sieve Nanomaterials (pages 805–809)

      X.-F. Shen, Y.-S. Ding, J. Liu, J. Cai, K. Laubernds, R. P. Zerger, A. Vasiliev, M. Aindow and S. L. Suib

      Article first published online: 30 MAR 2005 | DOI: 10.1002/adma.200401225

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      Manganese oxide octahedral molecular sieves with increasing nanoscale tunnel sizes are systematically synthesized using hydrothermal treatment of Na-birnessite under increasing pH conditions. OMS-5 (2×4), OMS-6 (2×3), and OMS-7 (1×1; see Figure) tunnel structures have been synthesized at pH values of 13, 7.0, and 1.0, respectively.

    5. Biologically Active Protein Gradients via Microstamping (pages 809–813)

      S. M. Bhangale, V. Tjong, L. Wu, N. Yakovlev and P. M. Moran

      Article first published online: 30 MAR 2005 | DOI: 10.1002/adma.200400547

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      Protein gradients on substrates are prepared using a microstamping technique. An Au pattern is transferred from a patterned silicon stamp to a polymeric substrate, and exposed polymer regions are then selectively activated for protein immobilization. The protein gradient is achieved by varying the spacing between the exposed polymer regions (see Figure).

    6. Organic Dye for Highly Efficient Solid-State Dye-Sensitized Solar Cells (pages 813–815)

      L. Schmidt-Mende, U. Bach, R. Humphry-Baker, T. Horiuchi, H. Miura, S. Ito, S. Uchida and M. Grätzel

      Article first published online: 30 MAR 2005 | DOI: 10.1002/adma.200401410

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      The feasibility of solid-state dye-sensitized solar cells as a low-cost alternative to amorphous silicon cells is demonstrated. Such a cell (see Figure) with a record efficiency of over 4 % under simulated sunlight is reported, made possible by using a new organic metal-free indoline dye (see Figure) as the sensitizer with high absorption coefficient.

    7. Towards Protein Field-Effect Transistors: Report and Model of a Prototype (pages 816–822)

      G. Maruccio, A. Biasco, P. Visconti, A. Bramanti, P. P. Pompa, F. Calabi, R. Cingolani, R. Rinaldi, S. Corni, R. Di Felice, E. Molinari, M. P. Verbeet and G. W. Canters

      Article first published online: 30 MAR 2005 | DOI: 10.1002/adma.200400628

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      A protein field-effect transistor (Pro-FET) based on the blue-copper protein azurins (see Figure) and operating at room temperature and ambient pressure is demonstrated. The transfer characteristics of the Pro-FET exhibit a pronounced resonance due to the switch from behaving as a n-metal oxide semiconductor FET (n-MOSFET) to a p-MOSFET. Carrier transport through the device is explained in terms of an equilibrium between the two possible oxidation states of the redox site (Cu1+ and Cu2+).

    8. Novel Light-Emitting Diodes Using Organic Electroluminescent Nanocapsules (pages 822–826)

      J.-S. Heo, N.-H. Park, J.-H. Ryu and K.-D. Suh

      Article first published online: 30 MAR 2005 | DOI: 10.1002/adma.200400051

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      Novel light-emitting diodes have been constructed using electroluminescent nanocapsules (ELCs) as the emitting layer (see Figure). The ELCs comprise electroluminescent perylene as a core with electron- and hole-transfer moieties in a polymeric shell, and were prepared by emulsion copolymerization, a technique that allows the properties of devices to be tuned via the appropriate selection of matrix polymer and other components.

    9. Magnetic Resonance Signal-Enhancing Self-Assembled Coating for Endovascular Devices (pages 826–830)

      B. Thierry, S. Faghihi, L. Torab, G. B. Pike and M. Tabrizian

      Article first published online: 30 MAR 2005 | DOI: 10.1002/adma.200401115

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      Magnetic resonance imaging (MRI) signal enhancement is reported using a coating grown by layer-by-layer assembly. A macromolecular conjugate of hyaluronan with Gd-coordinated diethylenetriaminepentaacetic acid is used with chitosan to coat polymeric interventional tools. The MRI visibility of such Gd-loaded coatings can be easily tailored by varying the number of layers (see Figure).

    10. A New Y3Al5O12 Phase Produced by Liquid-Feed Flame Spray Pyrolysis (LF-FSP) (pages 830–833)

      R. M. Laine, J. Marchal, H. Sun and X. Q. Pan

      Article first published online: 30 MAR 2005 | DOI: 10.1002/adma.200401001

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      Liquid-feed flame spray pyrolysis allows the synthesis of 20 nm diameter hexagonal Y3Al5O12 nanopowders (see Figure) that show no evidence of a yttrium aluminum garnet (YAG) phase. The nanopowders can be easily formed into green bodies that sinter to the YAG phase at nearly full density. This novel material offers potential for making high-quality YAG materials including ceramic lasers with exceptional control of processing parameters.

    11. Prefluorescent-Dye-Induced, Chemically Reversible Fluorescent Imaging Based on a Polymeric Photobase Generator (pages 833–837)

      W. S. Choi, Y.-Y. Noh and K. H. Chae

      Article first published online: 30 MAR 2005 | DOI: 10.1002/adma.200400841

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      A new method for fluorescence imaging based on a polymeric photobase generator containing oxime-urethane groups was developed via the use of fluorescamine, a prefluorescent amino-group dye. The fluorescent image obtained is stable and has a high contrast and good resolution (see Figure). In addition, it is possible that the fluorescent image can be erased or restored by the alternative treatment of base and acid.

    12. Ultrasound-Aided Remarkably Fast Assembly of Monolayers of Zeolite Crystals on Glass with a Very High Degree of Lateral Close Packing (pages 837–841)

      J. S. Lee, K. Ha, Y.-J. Lee and K. B. Yoon

      Article first published online: 30 MAR 2005 | DOI: 10.1002/adma.200401457

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      Strong ultrasonic agitation leads to more than a 103-fold increase in the rate of attachment of zeolite microcrystal monolayers to glass with molecular linkages compared to the rate by reflux and stirring. The degree of close packing also increases tremendously (see Figure).

    13. Self-Assembly and Micropatterning of Spherical-Particle Assemblies (pages 841–845)

      Y. Masuda, T. Itoh and K. Koumoto

      Article first published online: 10 FEB 2005 | DOI: 10.1002/adma.200400576

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      Spherical-particle assemblies (see Figure) are fabricated by micropatterning of methanol droplets containing SiO2. Hydrophilic regions of a patterned self-assembled monolayer (SAM) are covered with methanol solution containing SiO2 particles and immersed in decahydronaphthalene. The particles assemble to form micropatterns of spherical-particle assemblies on the hydrophilic regions of the SAM.

    14. Tunable Luminescence from a Silicon-Rich Oxide Microresonator (pages 845–849)

      A. Hryciw, J. Laforge, C. Blois, M. Glover and A. Meldrum

      Article first published online: 18 FEB 2005 | DOI: 10.1002/adma.200401230

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      Wide-wavelength tunability, from the blue to the near-infrared spectral regions, and spectrally narrow emission are achieved by embedding a silicon-rich oxide thin film in an optical microcavity structure. The low processing temperatures for these devices suggest compatibility with complementary metal oxide semiconductor fabrication techniques, indicating the potential of this material for integrated optoelectronic applications.

    15. Novel Peripherally Substituted Indolo[3,2-b]carbazoles for High-Mobility Organic Thin-Film Transistors (pages 849–853)

      Y. Li, Y. Wu, S. Gardner and B. S. Ong

      Article first published online: 30 MAR 2005 | DOI: 10.1002/adma.200401290

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      Strategically functionalized 5,11-dialkylindolo[3,2-b]carbazoles (see Figure) represent a novel class of high-mobility p-channel semiconductors for organic thin-film transistors. Specifically, 2,8-dichloro-substituted 5,11-didodecylindolo[3,2-b]carbazole, which forms highly crystalline films with large interconnecting terrace-like layered domain structures, has exhibited mobilities reaching 0.14 cm2 V–1 s–1 and current on/off ratios of 107 under ambient conditions.

    16. Fluorescent Nanocrystal–Polymer Complexes with Flexible Processability (pages 853–857)

      H. Zhang, C. Wang, M. Li, J. Zhang, G. Lu and B. Yang

      Article first published online: 30 MAR 2005 | DOI: 10.1002/adma.200401303

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      A simple process was developed to prepare fluorescent nanocrystal–polymer complexes with flexible processability. From these complexes one may facilely fabricate macroscopic fluorescent bulk in different shapes and fluorescent microspheres. The Figure is a photoluminescene image of the resultant composites.

    17. A Novel Transparent Vanadate Glass for Use in Fiber Optics (pages 857–859)

      B. Peng, Z. Fan, X. Qiu, L. Jiang, G. H. Tang, H. D. Ford and W. Huang

      Article first published online: 30 MAR 2005 | DOI: 10.1002/adma.200401271

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      Traditional vanadate glasses are known to be totally black (see inset Figure), while their crystal counterparts are promising laser materials due to their large stimulated-emission cross-section. In this work, a novel transparent vanadate glass (see main Figure) is realized for the first time. Furthermore, when doped with neodymium, its large stimulated-emission cross-section and low phonon energy demonstrate potential to be utilized in optical applications, especially in laser-related fiber optics.

    18. Preparation of Boron-Carbide/Carbon Nanofibers from a Poly(norbornenyldecaborane) Single-Source Precursor via Electrostatic Spinning (pages 859–862)

      D. T. Welna, J. D. Bender, X. Wei, L. G. Sneddon and H. R. Allcock

      Article first published online: 30 MAR 2005 | DOI: 10.1002/adma.200401257

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      Pyrolysis of poly(norbornenyldecaborane) that has been electrostatically spun provides a route to non-woven mats of boron-carbide/carbon ceramic nanofibers with narrow distributions and controllable dimensions (see Figure). This approach allows the fabrication of composite ceramic fibers with varying composition, which could be tailored to suit specific applications.

    19. Lithium-Ion Intercalation into TiO2-B Nanowires (pages 862–865)

      A. R. Armstrong, G. Armstrong, J. Canales, R. García and P. G. Bruce

      Article first published online: 30 MAR 2005 | DOI: 10.1002/adma.200400795

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      Li+ Intercalation into TiO2-B nanowires is reported up to a composition of Li0.91TiO2-B (specific charge capacity: 305 mA h g–1) and with a superior rate capability to nanoparticulate anatase and bulk TiO2-B (see Figure). The combination of high capacity for Li+ intercalation, high rate capability, and a potential of ∼1.6 V, renders the intercalated nanowires interesting as anodes for rechargeable lithium batteries and negative electrodes for supercapacitors.

    20. Highly Ultramicroporous Single-Walled Carbon Nanohorn Assemblies (pages 866–870)

      C.-M. Yang, H. Noguchi, K. Murata, M. Yudasaka, A. Hashimoto, S. Iijima and K. Kaneko

      Article first published online: 30 MAR 2005 | DOI: 10.1002/adma.200400712

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      Highly ultramicroporous single-walled carbon nanohorns (see Figure), porosity-designed by HNO3 treatment, show dramatically enhanced storage capacity of supercritical methane, which can be adsorbed into internal and interstitial spaces of the single-wall carbon nanohorns. This enhanced storage capacity of methane may result from the developed ultramicroporosity, which can promote the adsorptivity of methane.

    21. Novel Photoactive Single-Walled Carbon Nanotube–Porphyrin Polymer Wraps: Efficient and Long-Lived Intracomplex Charge Separation (pages 871–875)

      D. M. Guldi, H. Taieb, G. M. A. Rahman, N. Tagmatarchis and M. Prato

      Article first published online: 30 MAR 2005 | DOI: 10.1002/adma.200400641

      Thumbnail image of graphical abstract

      Novel donor-acceptor nanoassemblies (see cover) are prepared using pristine single-walled carbon nanotubes (SWNTs) as electron-acceptor components in supramolecular “polymer wraps”, with poly(methyl methacrylate) carrying porphyrin units (H2P) as excited-state electron donors (see Figure). In these novel donor–acceptor ensembles, SWNTs quench the photoexcited H2P chromophores, resulting in the creation of long-lived radical ion pairs.

    22. Fluorinated Naphthalocyanines Displaying Simultaneous Reverse Saturable Absorption at 532 and 1064 nm (pages 875–879)

      G. Y. Yang, M. Hanack, Y. W. Lee, D. Dini and J. F. Pan

      Article first published online: 30 MAR 2005 | DOI: 10.1002/adma.200401621

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      Photostable naphthalocyanines (see Figure) can act as optical limiters, simultaneously absorbing nanosecond laser pulses at 532 nm and 1064 nm. In these naphthalocyanines, where M can correspond to Zn, InCl, or In(p-trifluoromethylphenyl), the pattern of substitution and the nature of the substituents were found to be critical factors in achieving such a combination of linear and nonlinear optical properties.

    23. Colloidal Photonic Crystal with Graded Refractive-Index Distribution (pages 879–885)

      J.-H. Park, W. S. Choi, H. Y. Koo and D.-Y. Kim

      Article first published online: 30 MAR 2005 | DOI: 10.1002/adma.200400632

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      A photonic crystal structure with a refractive index that gradually changes in the specific direction of the crystal is demonstrated (see Figure). The colloidal photonic crystal was obtained by infiltration of a monomer and organic dopant with a high refractive index into the colloidal opal, followed by interfacial gel polymerization. The resulting colloidal crystal has a gradually varying stop-band at different positions in the crystal when the incident light is normal to the {111} crystallographic axis.

    24. Multiply Shaped Silica Mediated by Aggregates of Linear Poly(ethyleneimine) (pages 885–888)

      J.-J. Yuan and R.-H. Jin

      Article first published online: 30 MAR 2005 | DOI: 10.1002/adma.200401670

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      A new method for biomimetic silica fabrication is reported. Organized poly(ethyleneimine) rapidly catalyzes and directs the shape of silica in the hydrolysis of tetramethoxysilane under ambient conditions. The resultant silica displays a diversity of controllable morphologies, such as flower, plate, bundle, leaf, and sphere (see Figure, scale bar represents 1 μm).

    25. Bioleaching of Sand by the Fungus Fusarium oxysporum as a Means of Producing Extracellular Silica Nanoparticles (pages 889–892)

      V. Bansal, A. Sanyal, D. Rautaray, A. Ahmad and M. Sastry

      Article first published online: 30 MAR 2005 | DOI: 10.1002/adma.200401176

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      A plant pathogenic fungus, Fusarium oxysporum, can be used as a biological model system for the extracellular bioleaching of hollow spherical silica nanoparticles (see Figure) from sand. The room-temperature synthesis of oxide nanomaterials using microorganisms starting from potential waste materials could lead to eco-friendly and economically viable methods for the large-scale synthesis of nanomaterials.

    26. Microarrays of Peptide Fibrils Created by Electrostatically Controlled Deposition (pages 893–897)

      P. Mesquida, D. L. Ammann, C. E. MacPhee and R. A. McKendry

      Article first published online: 10 FEB 2005 | DOI: 10.1002/adma.200401229

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      The adsorption of β-sheet-rich fibrils produced in vitro via the self-assembly of polypeptides onto surfaces is found to be governed by electrostatic interactions. Chemically patterned substrates are used to create lateral micropatterns of fibrils and hybrid microstructures of fibrils with inorganic nanoparticles (see Figure). β-sheet-rich fibrils are promising as functional biomaterials.

    27. The Unusual Effect of Bandgap Lowering by C60 on a Conjugated Polymer (pages 897–900)

      G. Sonmez, C. K. F. Shen, Y. Rubin and F. Wudl

      Article first published online: 30 MAR 2005 | DOI: 10.1002/adma.200306494

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      Polymers with lowered bandgaps (see Figure) are produced from monomers containing a bisfulleroid as an electron-acceptor and thiophene as an electron-donor, fused by a thieno[3,4-b]pyrazine bridge. The bandgaps could reach as low as 0.25 eV. Electron flow from the poly(thiophene) backbone to the fullerene through the covalently bound thieno[3,4-b]pyrazine unit in the ground state makes this polymer a good candidate for the fabrication of photovoltaics and photoconductors.

    28. Synthesis and Reactivity of a Super-Reactive Metastable Intermolecular Composite Formulation of Al/KMnO4 (pages 900–903)

      A. Prakash, A. V. McCormick and M. R. Zachariah

      Article first published online: 30 MAR 2005 | DOI: 10.1002/adma.200400853

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      A new metastable intermolecular composite (MIC) which employs KMnO4 nanoparticles as the oxidizer has been developed for energetic-material applications. The nanoparticles are synthesized by a spray-drying process, and a strong correlation between pressurization rates (measurement schematic shown in Figure) for several MIC combinations and the fraction of reactive oxygen present in the combustion product is observed.

    29. Thickness-Driven Orthorhombic to Triclinic Phase Transformation in Pentacene Thin Films (pages 903–907)

      L. F. Drummy and D. C. Martin

      Article first published online: 30 MAR 2005 | DOI: 10.1002/adma.200400189

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      Pentacene films are thermally evaporated onto amorphous carbon-coated mica substrates held at room temperature. The crystal structure and morphology of the films are analyzed using electron microscopy and diffraction, and a new orthorhombic structure is characterized for films below a critical thickness (see Figure). Evidence that the orthorhombic structure is thermodynamically stable at low film thickness due to its low (001) surface energy is obtained.

    30. Polymer-Assisted Hydrothermal Synthesis of Single-Crystalline Tetragonal Perovskite PbZr0.52Ti0.48O3 Nanowires (pages 907–910)

      G. Xu, Z. Ren, P. Du, W. Weng, G. Shen and G. Han

      Article first published online: 30 MAR 2005 | DOI: 10.1002/adma.200400998

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      Single-crystalline nanorods and nanowires are grown using a hydrothermal system with the assistance of polymer additives. Tetragonal perovskite PbZr0.52Ti0.48O3 nanorods (see Figure) are grown in the presence of poly(vinyl alcohol), while nanowires are formed in the presence of poly(vinyl alcohol) and poly(acrylic acid). The polymers are absorbed on the axial side of the particles, reducing the surface energy and inducing oriented growth.

    31. New Composite MoS2–C60 Crystals (pages 911–914)

      M. Remškar, A. Mrzel, A. Jesih, J. Kovač, H. Cohen, R. Sanjinés and F. Lévy

      Article first published online: 30 MAR 2005 | DOI: 10.1002/adma.200400553

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      New MoS2–C60 composite layered crystals built of alternating MoS2 and C60 molecular layers and with unusual diffraction contrast (see Figure) have been grown via a catalyzed transport reaction using fullerene C60. A model structure of these layered composites is proposed based on transmission electron microscopy, electron diffraction, X-ray diffraction, and photoelectron spectroscopy. A growth mechanism is proposed based on electrostatic interactions, considering optical absorption by MoS2 and possible charge transfer to C60.

    32. Submicrometer Laminated Fe/SiO2 Soft Magnetic Composites—An Effective Route to Materials for High-Frequency Applications (pages 915–918)

      Y.-W. Zhao, X. K. Zhang and J. Q. Xiao

      Article first published online: 30 MAR 2005 | DOI: 10.1002/adma.200401096

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      Submicrometer laminated Fe/SiO2 soft magnetic composites (see Figure) have been fabricated by controlled deformation and subsequent sol–gel coating processes. The bulk materials made of these laminates show flat permeability spectra up to 50 MHz, about two orders of magnitude higher than those made of the parent powders. In addition, the composites have large saturation fields, and thus can be used in high-power devices.

    33. New, Highly Ion-Conductive Crystals Precipitated from Li2S–P2S5 Glasses (pages 918–921)

      F. Mizuno, A. Hayashi, K. Tadanaga and M. Tatsumisago

      Article first published online: 30 MAR 2005 | DOI: 10.1002/adma.200401286

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      Novel sulfide lithium-ion conducting materials are synthesized by crystallization of mechanically milled Li2S–P2S5 glasses. High ambient-temperature conductivities (σ) compared with other electrolytes (see Figure) and a low conduction activation energy are achieved by the formation of a highly conductive new crystalline phase.

    34. Biorelevant Calcification and Non-Cytotoxic Behavior in Silicon Nanowires (pages 921–924)

      D. K. Nagesha, M. A. Whitehead and J. L. Coffer

      Article first published online: 30 MAR 2005 | DOI: 10.1002/adma.200401362

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      Silicon nanowires develop a uniform synthetic bone coating under an electric-field bias in simulated body fluid. The hydroxyapatite-coated nanowires (see Figure) support fibroblast attachment and proliferation, and remain responsive to electrical bias even after coating, providing a system for electric-field modulated tissue regeneration.

    35. Synthesis of Monodisperse Colloidal Spheres, Capsules, and Microballoons by Emulsion Templating (pages 924–928)

      C. I. Zoldesi and A. Imhof

      Article first published online: 10 FEB 2005 | DOI: 10.1002/adma.200401183

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      New types of monodisperse, micrometer-sized, hollow particles (see Figure) are obtained by encapsulation of emulsion droplets in solid shells and dissolution of the cores. A facile fabrication method is used in which, by simply tuning the thickness of the shells, different types of particles with tunable properties are obtained.

    36. Fabrication of Ruthenium–Carbon Nanotube Nanocomposites in Supercritical Water (pages 928–932)

      Z. Sun, Z. Liu, B. Han, Y. Wang, J. Du, Z. Xie and G. Han

      Article first published online: 30 MAR 2005 | DOI: 10.1002/adma.200400839

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      Metal nanoparticles on carbon nanotubes (CNTs) are expected to be efficient catalysts for several industrially important processes. Here, the successful preparation of well-dispersed Ru–CNT nanocomposites—which are subsequently demonstrated to be very active for the hydrogenation of benzene to cyclohexane—using RuCl3·H2O as the precursor is reported. The Figure shows a transmission electron microscopy image of nano- composites used four times as a catalyst.

    37. Author Index and Subject Index Adv. Mater. 7/2005 (pages 933–934)

      Article first published online: 30 MAR 2005 | DOI: 10.1002/adma.200590035

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