Advanced Functional Materials

Cover image for Vol. 22 Issue 21

November 7, 2012

Volume 22, Issue 21

Pages 4401–4619

  1. Cover Picture

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    1. Graphene: Spongy Graphene as a Highly Efficient and Recyclable Sorbent for Oils and Organic Solvents (Adv. Funct. Mater. 21/2012) (page 4401)

      Hengchang Bi, Xiao Xie, Kuibo Yin, Yilong Zhou, Shu Wan, Longbing He, Feng Xu, Florian Banhart, Litao Sun and Rodney S. Ruoff

      Version of Record online: 2 NOV 2012 | DOI: 10.1002/adfm.201290127

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      Spongy graphene (SG), a nanoporous material with a high surface area, is used as a versatile and recyclable sorber. On page 4421, Litao Sun, Rodney S. Ruoff, and co-workers report that SG shows highly efficient absorption of petroleum products, fats, and toxic solvents and can be regenerated by heat treatment, yielding almost full release of the adsorbates. SG shows a widespread potential for applications in industry and environmental protection.

  2. Inside Front Cover

    1. Top of page
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    5. Masthead
    6. Contents
    7. Full Papers
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    1. Surface Characterization: Non-Invasive High-Throughput Metrology of Functionalized Graphene Sheets (Adv. Funct. Mater. 21/2012) (page 4402)

      Maziar Ghazinejad, Jennifer Reiber Kyle, Shirui Guo, Dennis Pleskot, Duoduo Bao, Valentine I. Vullev, Mihrimah Ozkan and Cengiz S. Ozkan

      Version of Record online: 2 NOV 2012 | DOI: 10.1002/adfm.201290128

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      On page 4519, Mihrimah Ozkan, Cengiz S. Ozkan, and co-workers report a new fluorescence quenching microscopy metrology technique that allows the identification of graphene layers and doped/undoped regions across a large graphene landscape by utilizing the fact that undoped regions of graphene quench fluorescence more than the doped regions through resonant energy transfer. Contrast differences in fluorescence across the graphene sheet reveal the complex ring-patterned doping. This metrology technique is well-suited for industrial, large-scale, pristine, and modified graphene sheet surface characterization.

  3. Back Cover

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    1. Spintronics: Large Tunnel Magnetoresistance in Epitaxial Oxide Spin-Filter Tunnel Junctions (Adv. Funct. Mater. 21/2012) (page 4620)

      Takayuki Harada, Isao Ohkubo, Mikk Lippmaa, Yasuaki Sakurai, Yuji Matsumoto, Shunsuke Muto, Hideomi Koinuma and Masaharu Oshima

      Version of Record online: 2 NOV 2012 | DOI: 10.1002/adfm.201290129

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      A spin-polarized-current generator is a fundamental device in spintronics. As reported on page 4471, Isao Ohkubo and co-workers have developed a highperformance spin-filter tunnel junction by growing an atomic-layer-controlled oxide multilayer. In this device, up-spin electrons can selectively tunnel through a nanometer-thick ferromagnetic insulator, while down-spin electrons are reflected. The image shows a false-colored cross-sectional transmission electron microscope image of the device.

  4. Masthead

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    1. Masthead: (Adv. Funct. Mater. 21/2012)

      Version of Record online: 2 NOV 2012 | DOI: 10.1002/adfm.201290130

  5. Contents

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  6. Full Papers

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    1. Osteoconductive Performance of Carbon Nanotube Scaffolds Homogeneously Mineralized by Flow-Through Electrodeposition (pages 4411–4420)

      Stefania Nardecchia, M. Concepción Serrano, María C. Gutiérrez, M. Teresa Portolés, M. Luisa Ferrer and Francisco del Monte

      Version of Record online: 20 JUN 2012 | DOI: 10.1002/adfm.201200684

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      Coating the entire internal surface of “true” 3D scaffolds with a homogeneous mineral layer is by no means a trivial issue. This problem is overcome by the application of a “flow-through” electrodeposition process to scaffolds composed of multiwall carbon nanotubes and chitosan. The scaffolds resulting after mineralization exhibit a remarkable biocompatibility and superior osteoconductive performance.

    2. Spongy Graphene as a Highly Efficient and Recyclable Sorbent for Oils and Organic Solvents (pages 4421–4425)

      Hengchang Bi, Xiao Xie, Kuibo Yin, Yilong Zhou, Shu Wan, Longbing He, Feng Xu, Florian Banhart, Litao Sun and Rodney S. Ruoff

      Version of Record online: 20 JUN 2012 | DOI: 10.1002/adfm.201200888

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      Spongy graphene (SG) shows highly efficient absorption of not only petroleum products and fats but also common toxic solvents such as toluene and chloroform, taking in up to 86 times its own weight. This is several to tens of times higher than that of conventional absorbers. Moreover, the SG can be regenerated more than ten times by heat treatment yielding the full release of adsorbates.

    3. A Universal Molecular Stent Method to Toughen any Hydrogels Based on Double Network Concept (pages 4426–4432)

      Tasuku Nakajima, Hitomi Sato, Yu Zhao, Shinya Kawahara, Takayuki Kurokawa, Kazuyuki Sugahara and Jian Ping Gong

      Version of Record online: 20 JUN 2012 | DOI: 10.1002/adfm.201200809

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      Tough hydrogels can be synthesized from any hydrophilic polymer by the double-network (DN) concept using a molecular stent. The synthesized St-DN gels have excellent strength and toughness comparable to those of conventional tough DN gels and industrial rubbers. This is a promising method for strengthening various functional hydrogels and increasing the scope of their application in various fields.

    4. Photocatalytic Composites of Silicone Nanofilaments and TiO2 Nanoparticles (pages 4433–4438)

      Georg R. Meseck, Roman Kontic, Greta R. Patzke and Stefan Seeger

      Version of Record online: 26 JUN 2012 | DOI: 10.1002/adfm.201200816

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      A new strategy for the immobilization of nanoscale TiO2 photocatalysts is presented via their growth on carpets of silicone nanofilaments. These nanofilaments are novel and flexible carrier prototypes for the safe and recyclable application of TiO2 nanocatalysts. Their compatibility with various surfaces and their functionalization options open up new avenues for photocatalyst design.

    5. Linewidth-Optimized Extraordinary Optical Transmission in Water with Template-Stripped Metallic Nanohole Arrays (pages 4439–4446)

      Si Hoon Lee, Timothy W. Johnson, Nathan C. Lindquist, Hyungsoon Im, David J. Norris and Sang-Hyun Oh

      Version of Record online: 3 JUL 2012 | DOI: 10.1002/adfm.201200955

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      An extraordinary optical transmission peak in water with a linewidth of 9.9 nm and a Q factor of 71 is demonstrated via template-stripped metallic nanohole arrays with a surface roughness below 1 nm and a precisely tuned hole size. The nanostructured films exhibit extremely uniform optical properties across a centimeter-sized area and enable a series of practical applications in biosensing and spectroscopy.

  7. Frontispiece

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    1. Cell Separation: Ethanol-Dispersed Polymer Nanofibers as a Highly Selective Cell Isolation and Release Platform for CD4+ T Lymphocytes (Adv. Funct. Mater. 21/2012) (page 4447)

      Seung-Hyun Jun, Kwanghee Kim, Hyo Jin An, Byoung Chan Kim, Chung Hee Sonn, Miju Kim, Junsang Doh, Cassian Yee, Kyung-Mi Lee and Jungbae Kim

      Version of Record online: 2 NOV 2012 | DOI: 10.1002/adfm.201290125

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      Electrospun and alcohol-dispersed polystyrene-poly(styreneco-maleic anhydride) (PS-PSMA) nanofibers, which allow for facile conjugation of antibodies, are used as an innovative cell isolation/enrichment and support/release platform. As reported by Kyung-Mi Lee, Jungbae Kim, and co-workers on page 4448, this work opens up the potential for an innovative immune cell therapy in which specific immune cells are isolated by antibody-conjugated nanofibers and are directly delivered to the target sites under the controlled and sustained release of immune cells via in vivo activation.

  8. Full Papers

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    1. Ethanol-Dispersed Polymer Nanofibers as a Highly Selective Cell Isolation and Release Platform for CD4+ T Lymphocytes (pages 4448–4455)

      Seung-Hyun Jun, Kwanghee Kim, Hyo Jin An, Byoung Chan Kim, Chung Hee Sonn, Miju Kim, Junsang Doh, Cassian Yee, Kyung-Mi Lee and Jungbae Kim

      Version of Record online: 25 JUN 2012 | DOI: 10.1002/adfm.201200657

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      Electrospun and alcohol-dispersed PS-PSMA nanofibers, allowing for facile conjugation of antibodies, could be used as an innovative cell isolation/enrichment and support/release platform. This work opens up a new potential for an innovative immune cell therapy, in which specific immune cells are isolated by antibody-conjugated nanofibers and directly delivered to the target disease sites under the controlled and sustained release of immune cells via in vivo activation.

    2. Proton Conducting Phase-Separated Multiblock Copolymers with Sulfonated Poly(phenylene sulfone) Blocks for Electrochemical Applications: Preparation, Morphology, Hydration Behavior, and Transport (pages 4456–4470)

      Giorgi Titvinidze, Klaus-Dieter Kreuer, Michael Schuster, Carla C. de Araujo, Jan P. Melchior and Wolfgang H. Meyer

      Version of Record online: 25 JUN 2012 | DOI: 10.1002/adfm.201200811

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      Phase-separated multiblock copolymers are quite ordinary, but this is not so if they are based on fully sulfonated polysulfones as the hydrophilic segments. The aromatic sulfone structure gives rise to high chemical and thermal stability, while the hydrophilic domain structure allows for high proton conductivity with low hydrodynamic water transport. Such membranes have the potential to substitute traditional perfluorosulfonic acid (PFSA) membranes in fuel cells.

    3. Large Tunnel Magnetoresistance in Epitaxial Oxide Spin-Filter Tunnel Junctions (pages 4471–4475)

      Takayuki Harada, Isao Ohkubo, Mikk Lippmaa, Yasuaki Sakurai, Yuji Matsumoto, Shunsuke Muto, Hideomi Koinuma and Masaharu Oshima

      Version of Record online: 2 JUL 2012 | DOI: 10.1002/adfm.201200985

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      An epitaxial oxide spin-filter tunnel junction is fabricated by pulsed laser deposition with atomic-layer precision. By cutting magnetic coupling at a spin filter/spin detector interface, clear tunnel magnetoresistance exceeding 120% is obtained. The composition-controlled magnetic hardness of a Pr0.8Ca0.2Mn1-yCoyO3 spin filter layer makes it possible to develop an epitaxial double spin filter tunnel junction.

    4. Active, Programmable Elastomeric Surfaces with Tunable Adhesion for Deterministic Assembly by Transfer Printing (pages 4476–4484)

      Andrew Carlson, Shuodao Wang, Paulius Elvikis, Placid M. Ferreira, Yonggang Huang and John A. Rogers

      Version of Record online: 20 JUN 2012 | DOI: 10.1002/adfm.201201023

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      Active, programmable control of interfacial adhesion is an important, desired feature of many existing and envisioned systems, including medical tapes, releasable joints, and stamps for transfer printing. A design for an elastomeric surface that offers tunable adhesion strength through a combination of peel-rate dependent effects and actuation of subsurface fluid chambers is presented. When implemented in stamps for transfer printing, these structures provide utility in deterministic assembly of micro- and nanoscale materials onto diverse types of substrates including plastic, paper, and even the living surfaces of leaves.

    5. Smart Polymeric Cathode Material with Intrinsic Overcharge Protection Based on a 2,5-Di-tert-butyl- 1,4-dimethoxybenzene Core Structure (pages 4485–4492)

      Wei Weng, Zhengcheng Zhang, Ali Abouimrane, Paul C. Redfern, Larry A. Curtiss and Khalil Amine

      Version of Record online: 25 JUN 2012 | DOI: 10.1002/adfm.201200458

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      A new polymeric cathode (I) based on a redox shuttle (RS) core displays reversible oxidation/reduction at ≈3.96 V vs Li/Li+. At a 1C rate, the polymer I/Li cell shows stable cycling up to 200 cycles between 4.05 and 3.0 V with less than 10% capacity loss. When overcharged, an intrinsic RS mechanism is remarkably activated at 4.2 V.

    6. A Natural Silk Fibroin Protein-Based Transparent Bio-Memristor (pages 4493–4499)

      Mrinal K. Hota, Milan K. Bera, Banani Kundu, Subhas C. Kundu and Chinmay K. Maiti

      Version of Record online: 3 JUL 2012 | DOI: 10.1002/adfm.201200073

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      A silk fibroin protein-based biomemristor demonstrates bipolar memristive switching, which can be explained using the concept of carrier trapping or detrapping in silk fibroin films due to a redox process. The rapid transition between oxidation and reduction states of silk in response to diverse applied electric fields significantly contributes to the memristive switching. This bioelectronics memory device opens up ample opportunities in neuromorphic computing, high-density logic, and memory applications.

  9. Frontispiece

    1. Top of page
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    1. Supercapacitors: Micro-Supercapacitors Based on Interdigital Electrodes of Reduced Graphene Oxide and Carbon Nanotube Composites with Ultrahigh Power Handling Performance (Adv. Funct. Mater. 21/2012) (page 4500)

      Majid Beidaghi and Chunlei Wang

      Version of Record online: 2 NOV 2012 | DOI: 10.1002/adfm.201290126

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      The design and fabrication of graphene-based micro-supercapacitors are reported on page 4501 by Majid Beidaghi and Chunlei Wang. Addition of carbon nanotubes (CNTs) between the graphene sheets and the arrangement of electrodes in a side-by-side structure increases the accessibility of electrode materials. A two-step fabrication of electrodes based on electrostatic spray deposition (ESD) and photolithography lift-off is explained. The fabricated devices show exceptional high rate capability and frequency response. Image courtesy of Kristy Jost.

  10. Full Papers

    1. Top of page
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    1. Micro-Supercapacitors Based on Interdigital Electrodes of Reduced Graphene Oxide and Carbon Nanotube Composites with Ultrahigh Power Handling Performance (pages 4501–4510)

      Majid Beidaghi and Chunlei Wang

      Version of Record online: 29 JUN 2012 | DOI: 10.1002/adfm.201201292

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      Binder-free micropatterned electrodes of reduced graphene oxide and carbon nanotube composites are prepared for micro-supercapacitor application by combining electrostatic spray deposition and photolithography lift-off. The high accessibility of the electrode materials and short diffusion path of electrolyte ions results in excellent rate capability and frequency response of the micro-supercapacitors.

    2. Integration of Self-Assembled Microvascular Networks with Microfabricated PEG-Based Hydrogels (pages 4511–4518)

      Michael P. Cuchiara, Daniel J. Gould, Melissa K. McHale, Mary E. Dickinson and Jennifer L. West

      Version of Record online: 20 JUN 2012 | DOI: 10.1002/adfm.201200976

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      The most significant tissue engineering barrier is insufficient vascularization. A microfluidic hydrogel is integrated with a self-assembling pro-vasculogenic co-culture to control vessel establishment and create an anastomotic interface for integration with fabricated microchannels. Vessel development is temporally regulated. It is further shown that transport within these regions shifts from diffusion to vessel-supported convective movement.

    3. Non-Invasive High-Throughput Metrology of Functionalized Graphene Sheets (pages 4519–4525)

      Maziar Ghazinejad, Jennifer Reiber Kyle, Shirui Guo, Dennis Pleskot, Duoduo Bao, Valentine I. Vullev, Mihrimah Ozkan and Cengiz S. Ozkan

      Version of Record online: 6 JUL 2012 | DOI: 10.1002/adfm.201200434

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      The utilization of fluorescence quenching microscopy (FQM) for quick visualization of chemical functionalization in relatively large regions of graphene is described. With premeditated choice of the dye, the interaction between fluorophores and graphene provides advantages for probing the chemical structure of functionalized graphene. Segmented FQM can be employed to address the chronic need for microscopy-based graphene metrology.

    4. “Ship-in-a-Bottle” Growth of Noble Metal Nanostructures (pages 4526–4532)

      Manda Xiao, Chunmei Zhao, Huanjun Chen, Baocheng Yang and Jianfang Wang

      Version of Record online: 29 JUN 2012 | DOI: 10.1002/adfm.201200941

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      Different monometallic Au and bimetallic Au-cored nanostructures are grown using a “ship-in-a-bottle” technique in hollow mesoporous silica microspheres. The microsphere-encapsulated Au nanorod core/Pt shell nanostructures exhibit both high catalytic performance and superior recyclability in the oxidation reaction of o-phenylenediamine with hydrogen peroxide, while the conversion percentage in the presence of the corresponding unencapsulated nanostructures decreases rapidly with the recycle number.

    5. Fabrication of Chemical Gradient Using Space Limited Plasma Oxidation and its Application for Droplet Motion (pages 4533–4538)

      Xiaojun Han, Lei Wang and Xuejing Wang

      Version of Record online: 19 JUN 2012 | DOI: 10.1002/adfm.201201121

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      A novel approach, space limited plasma oxidation, is introduced to fabricate chemical gradients on self-assembled monolayer (SAM) surfaces. This method is highly versatile, rapid, and low cost. It provides an easy way to fabricate gradient surfaces which can be either further functionalized by biomolecules (enzymes, antibodies, DNA, etc.) for investigation of biomolecular interactions, cell-adhesion studies and diagnostics, or used for spontaneous droplet motion.

    6. Enhancement of Proton Conduction at Low Humidity by Incorporating Imidazole Microcapsules into Polymer Electrolyte Membranes (pages 4539–4546)

      Jingtao Wang, Xiujun Yue, Zizhuo Zhang, Zheng Yang, Yifan Li, Han Zhang, Xinlin Yang, Hong Wu and Zhongyi Jiang

      Version of Record online: 25 JUN 2012 | DOI: 10.1002/adfm.201201436

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      Imidazole microcapsules with high imidazole group loading and large lumen size are synthesized and incorporated into a sulfonated poly(ether ether ketone) (SPEEK) membrane. Due to its superior water retention properties, anhydrous proton transfer feature of embedded imidazole microcapsules, and the low energy barrier pathways from the acid-base pairs, the SPEEK composite membrane displays notably enhanced proton conductivity in particular under low humidity.

    7. Dynamic Processes in Sandwich Polymer Light-Emitting Electrochemical Cells (pages 4547–4556)

      Stephan van Reenen, René A. J. Janssen and Martijn Kemerink

      Version of Record online: 25 JUN 2012 | DOI: 10.1002/adfm.201200880

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      Ion conductivity, electric double layer thickness, and electrochemical doping are identified by numerical modeling of admittance spectroscopy on light- emitting electrochemical cells (LECs). These results confirm the validity of the electrochemical doping model to describe LEC operation and it is shown that in order to significantly decrease the response-time of LECs an electrolyte/salt combination with a minimal ion binding energy must be used.

    8. Transition Metal Oxide Work Functions: The Influence of Cation Oxidation State and Oxygen Vacancies (pages 4557–4568)

      Mark T. Greiner, Lily Chai, Michael G. Helander, Wing-Man Tang and Zheng-Hong Lu

      Version of Record online: 26 JUN 2012 | DOI: 10.1002/adfm.201200615

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      The work functions of transition-metal oxides are correlated with the oxidation states of their metal cations. Due to the relationship between electronegativity and oxidation state, reduced oxides tend to have lower work functions. The trends revealed provide guidelines for tuning transition metal oxide work functions.

    9. Elaborately Aligning Bead-Shaped Nanowire Arrays Generated by a Superhydrophobic Micropillar Guiding Strategy (pages 4569–4576)

      Yuchen Wu, Xiao Chen, Bin Su, Yanlin Song and Lei Jiang

      Version of Record online: 25 JUN 2012 | DOI: 10.1002/adfm.201200971

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      Regularly aligning bead-shaped nanowire arrays are generated, assisted by highly adhesive superhydrophobic pillar- structured silicon substrates. The bead-shaped structures can be introduced by either Rayleigh instability at ultralow polymer concentration or rigid polystyrene spheres serving as bead building blocks. Furthermore, bead-shaped nanowires have the unique ability to directionally drive tiny drops and collect coalesced microdroplets when placed in mist.

    10. Optimal Structure for High-Performance and Low-Contact-Resistance Organic Field-Effect Transistors Using Contact-Doped Coplanar and Pseudo-Staggered Device Architectures (pages 4577–4583)

      Peter Darmawan, Takeo Minari, Yong Xu, Song-Lin Li, Haisheng Song, Meiyin Chan and Kazuhito Tsukagoshi

      Version of Record online: 21 JUN 2012 | DOI: 10.1002/adfm.201201094

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      An exceptionally low contact resistance is achieved in top-gated organic field-effect transistors by using coplanar and pseudo-staggered device architectures and introducing a dopant layer. Compared with conventional bottom-gated staggered devices, a remarkably low contact resistance is extracted from the top-gated devices by the modified transfer line method.

    11. Facile Synthesis of Manganese-Oxide-Containing Mesoporous Nitrogen-Doped Carbon for Efficient Oxygen Reduction (pages 4584–4591)

      Yueming Tan, Chaofa Xu, Guangxu Chen, Xiaoliang Fang, Nanfeng Zheng and Qingji Xie

      Version of Record online: 26 JUN 2012 | DOI: 10.1002/adfm.201201244

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      A novel MnO-containing mesoporous nitrogen-doped carbon (m-N-C) nanocomposite is facilely synthesized using an in situ manganese oxide template method. The MnO-m-N-C composite catalyst shows similar electrocatalytic activity but superior stability and methanol tolerance to a commercial Pt/C catalyst for the four-electron oxygen reduction reaction in alkaline solution.

    12. Ultrathin Mesoporous NiCo2O4 Nanosheets Supported on Ni Foam as Advanced Electrodes for Supercapacitors (pages 4592–4597)

      Changzhou Yuan, Jiaoyang Li, Linrui Hou, Xiaogang Zhang, Laifa Shen and Xiong Wen (David) Lou

      Version of Record online: 26 JUN 2012 | DOI: 10.1002/adfm.201200994

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      An advanced 3D self-supported electrode is fabricated by growing ultrathin mesoporous NiCo2O4 nanosheets on Ni foam with strong adhesion for high-performance electrochemical capacitors. Because of its many advantageous structural features, this self-supported hybrid electrode is able to deliver ultrahigh specific capacitance at a very high current density, with excellent cycling stability.

    13. Crystalline Organic Heterostructures Engineering Based on Vanadyl Phthalocyanine and Rod-Like Conjugated Organic Semiconductors with Selected Central Groups (pages 4598–4607)

      Lizhen Huang, Feng Zhu, Chengfang Liu, Uwe Treske, Mandy Grobosch, Hongkun Tian, Jidong Zhang, Yanhou Geng, Martin Knupfer and Donghang Yan

      Version of Record online: 20 JUN 2012 | DOI: 10.1002/adfm.201200014

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      Highly ordered organic crystals are is constructed from a series rod-like molecules and a disc-like phthalocyanine. The series of rod-like molecules differed in the central groups and present different lattice parameters and electronic structure, which results in distinct morphology and electronic structure in the heterostructure. Transistors based on the crystalline heterostructure present diverse charge transport behavior and field-effect mobilities.

    14. Recombination Through Different Types of Localized States in Organic Solar Cells (pages 4608–4619)

      Robert A. Street, Alexa Krakaris and Sarah R. Cowan

      Version of Record online: 3 JUL 2012 | DOI: 10.1002/adfm.201200031

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      Recombination in bulk heterojunction solar cells is explored by observing the results of extended white light illumination, thermal annealing to high temperature, and chemical doping. Measurements of spectral response and other cell characteristics show that recombination is through localized states of different type, depending on the circumstances.

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