ChemSusChem

Cover image for Vol. 8 Issue 8

April 24, 2015

Volume 8, Issue 8

Pages 1289–1491

  1. Cover Pictures

    1. Top of page
    2. Cover Pictures
    3. Cover Profile
    4. Graphical Abstract
    5. Corrigendum
    6. Masthead
    7. News
    8. Minireview
    9. Communications
    10. Full Papers
    1. You have free access to this content
      Cover Picture: Mechanism of Brønsted Acid-Catalyzed Glucose Dehydration (ChemSusChem 8/2015) (page 1289)

      Dr. Liu Yang, Dr. George Tsilomelekis, Dr. Stavros Caratzoulas and Dr. Dionisios G. Vlachos

      Article first published online: 16 APR 2015 | DOI: 10.1002/cssc.201500074

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      The Front Cover picture presents the DFT-based microkinetic model for the Brønsted acid-catalyzed conversion of glucose to 5-hydroxylmethyl furfural (HMF), levulinic acid, and formic acid. Isotopic tracing coupled with kinetic experiments provides a quantitative method to assess the mechanism and to propose unknown pathways among numerous ones that could be studied using first principles methods. We reveal that glucose dehydrates through a cyclic path, whereas the rate-limiting step is the first dehydration of protonated glucose and that the majority of glucose is consumed via the HMF intermediate. More details can be found in the Full Paper by Yang et al. on page 1334 (DOI: 10.1002/cssc.201403264).

    2. You have free access to this content
      Inside Cover: From Lignocellulosic Biomass to Lactic- and Glycolic-Acid Oligomers: A Gram-Scale Microwave-Assisted Protocol (ChemSusChem 8/2015) (page 1290)

      Diego Carnaroglio, Silvia Tabasso, Beata Kwasek, Dariusz Bogdal, Emanuela Calcio Gaudino and Giancarlo Cravotto

      Article first published online: 17 APR 2015 | DOI: 10.1002/cssc.201500278

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      The Inside Cover picture shows the complementary action of different microwave reactors in destroying the polymer chains of lignocellulosic biomass and rebuilding oligomers from the recovered building blocks. We designed a “microwave factory in the lab” for a flash catalytic conversion of biomass to selective platform chemicals—a sustainable protocol carried out in a microwave flow reactor. Lactic and glycolic acids were efficiently reacted to synthesize oligomers via a solvent- and catalyst-free microwave-assisted process under vacuum. Enabling technologies play a important role in biomass valorization, from agricultural wastes to value-added products in agreement with modern biorefinery. More details can be found in the Full Paper by Carnaroglio et al. on page 1342 (DOI: 10.1002/cssc.2014003183).

    3. You have free access to this content
      Inside Back Cover: Silver Phosphate/Graphitic Carbon Nitride as an Efficient Photocatalytic Tandem System for Oxygen Evolution (ChemSusChem 8/2015) (page 1493)

      Dr. Xiaofei Yang, Dr. Hua Tang, Dr. Jingsan Xu, Prof. Markus Antonietti and Dr. Menny Shalom

      Article first published online: 16 APR 2015 | DOI: 10.1002/cssc.201500464

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      The Inside Back Cover image shows the photo-oxidation of water using silver phosphate/carbon nitride (Ag3PO4/g-C3N4). While tremendous efforts into the development photocatalytically active materials afforded highly efficient H2 evolution catalysts, the complementary, water oxidation reaction (mechanistically more demanding) remains the major obstacle for overall water splitting. The composite material is superior in both efficiency and stability compared to pristine Ag3PO4 and C3N4. A detailed analysis of the reactions mechanism strongly implies the in situ formation of an effective Z-scheme (mimicking photosynthesis in nature) through formation of Ag nanoparticles at the material interface under illumination, which is different to the conventional charge transport through the interface; this opens a method for the preparation of catalysts for full water splitting systems and other uphill energy conversion reactions. More details can be found in the Full Paper by Yang et al. on page 1350 (DOI: 10.1002/cssc.201403168).

    4. Back Cover: Enhancing the Performance of a Robust Sol–Gel-Processed p-Type Delafossite CuFeO2 Photocathode for Solar Water Reduction (ChemSusChem 8/2015) (page 1494)

      Mathieu S. Prévot, Dr. Néstor Guijarro and Prof. Kevin Sivula

      Article first published online: 24 APR 2015 | DOI: 10.1002/cssc.201500316

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      The Back Cover picture shows a solution-processed thin film of semi-conducting CuFeO2 held in front of the sun. An impressive performance is reported using this material as a photocathode for the reduction of water molecules to hydrogen (as depicted in the bottom right corner) under solar radiation. In addition to being fully solution processable, the copper-based delafossite (crystal structure is shown in the top right corner) is a class of material known for being stable in aqueous environments. Moreover, it is only composed of earth-abundant materials, as suggested by the delafossite ore shown in the bottom right corner. Overall, these properties make p-type CuFeO2 a very attractive material in the quest for inexpensive, sustainable, and stable direct solar water splitting for the generation of carbon-free hydrogen. More details can be found in the Full Paper by Prévot et al. on page 1359 (DOI: 10.1002/cssc.201403146).

  2. Cover Profile

    1. Top of page
    2. Cover Pictures
    3. Cover Profile
    4. Graphical Abstract
    5. Corrigendum
    6. Masthead
    7. News
    8. Minireview
    9. Communications
    10. Full Papers
    1. Mechanism of Brønsted Acid-Catalyzed Glucose Dehydration (page 1291)

      Dr. Liu Yang, Dr. George Tsilomelekis, Dr. Stavros Caratzoulas and Dr. Dionisios G. Vlachos

      Article first published online: 17 APR 2015 | DOI: 10.1002/cssc.201500073

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      “Our research endeavours to target real-world, energy-related problems in an interdisciplinary environment….” This and more about the story behind the research that inspired the cover image is presented in the Cover Profile. More details can be found in the Full Paper by Yang et al.: 10.1002/cssc.201403264. View the Front Cover here: 10.1002/cssc.201500074.

  3. Graphical Abstract

    1. Top of page
    2. Cover Pictures
    3. Cover Profile
    4. Graphical Abstract
    5. Corrigendum
    6. Masthead
    7. News
    8. Minireview
    9. Communications
    10. Full Papers
    1. You have free access to this content
      Graphical Abstract: ChemSusChem 8/2015 (pages 1292–1299)

      Article first published online: 24 APR 2015 | DOI: 10.1002/cssc.201590014

  4. Corrigendum

    1. Top of page
    2. Cover Pictures
    3. Cover Profile
    4. Graphical Abstract
    5. Corrigendum
    6. Masthead
    7. News
    8. Minireview
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    1. You have free access to this content
      Corrigendum: Photogeneration of Hydrogen from Water by Hybrid Molybdenum Sulfide Clusters Immobilized on Titania (page 1299)

      David Recatalá, Prof. Rosa Llusar, Dr. Artem L. Gushchin, Dr. Ekaterina A. Kozlova, Yuliya A. Laricheva, Dr. Pavel A. Abramov, Prof. Maxim N. Sokolov, Prof. Roberto Gómez and Prof. Teresa Lana-Villarreal

      Article first published online: 14 APR 2015 | DOI: 10.1002/cssc.201500446

      This article corrects:

      Photogeneration of Hydrogen from Water by Hybrid Molybdenum Sulfide Clusters Immobilized on Titania

      Vol. 8, Issue 1, 148–157, Article first published online: 30 OCT 2014

  5. Masthead

    1. Top of page
    2. Cover Pictures
    3. Cover Profile
    4. Graphical Abstract
    5. Corrigendum
    6. Masthead
    7. News
    8. Minireview
    9. Communications
    10. Full Papers
    1. Masthead: ChemSusChem 8/2015 (pages 1300–1301)

      Article first published online: 24 APR 2015 | DOI: 10.1002/cssc.201590015

  6. News

    1. Top of page
    2. Cover Pictures
    3. Cover Profile
    4. Graphical Abstract
    5. Corrigendum
    6. Masthead
    7. News
    8. Minireview
    9. Communications
    10. Full Papers
  7. Minireview

    1. Top of page
    2. Cover Pictures
    3. Cover Profile
    4. Graphical Abstract
    5. Corrigendum
    6. Masthead
    7. News
    8. Minireview
    9. Communications
    10. Full Papers
    1. A Critical View on Catalytic Pyrolysis of Biomass (pages 1306–1316)

      Dr. R. H. Venderbosch

      Article first published online: 14 APR 2015 | DOI: 10.1002/cssc.201500115

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      The pitfalls of pyrolysis: Catalytic pyrolysis is seen as a promising route to yield liquids with a higher quality. However, in an initial stage of the catalytic process, reactive components are mainly converted to coke, gas, and water, and to a limited extent to a liquid product. Catalysts are not good enough, and finding ones to yield improved quality liquids may be practically impossible.

  8. Communications

    1. Top of page
    2. Cover Pictures
    3. Cover Profile
    4. Graphical Abstract
    5. Corrigendum
    6. Masthead
    7. News
    8. Minireview
    9. Communications
    10. Full Papers
    1. Solvent-Enabled Nonenyzmatic Sugar Production from Biomass for Chemical and Biological Upgrading (pages 1317–1322)

      Prof. Dr. Jeremy S. Luterbacher, Dr. David Martin Alonso, Jacqueline M. Rand, Ydna M. Questell-Santiago, Jher Hau Yeap, Prof. Dr. Brian F. Pfleger and Prof. Dr. James A. Dumesic

      Article first published online: 17 MAR 2015 | DOI: 10.1002/cssc.201403418

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      Super phenolic solvents: Biomass-derived carbohydrates represent an attractive source of renewable carbon due to their many chemical and biological conversion routes to fuels and chemicals. In a nonenzymatic biomass deconstruction process for producing carbohydrates, separating a mixture of γ-valerolactone (GVL) and water used in the process is a key step. We demonstrate that phenolic solvents are highly effective at separating GVL and can be used to detoxify the biomass-derived mixture for fermentation.

    2. Copper–Zinc Alloy Nanopowder: A Robust Precious-Metal-Free Catalyst for the Conversion of 5-Hydroxymethylfurfural (pages 1323–1327)

      Dr. Giovanni Bottari, Angela J. Kumalaputri, Dr. Krzysztof K. Krawczyk, Prof. Ben L. Feringa, Prof. Hero J. Heeres and Dr. Katalin Barta

      Article first published online: 1 APR 2015 | DOI: 10.1002/cssc.201403453

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      Revival of the ‘brass-age′: Commercially available copper–zinc nanopowder proves very robust and highly effective in the reduction of HMF to either fuel additives or useful chemical building blocks. Fuel yields of up to 97 % and FDM yield up to 95 % were obtained. The one-pot conversion of fructose to furanic diethers is also achieved, in isopropanol solvent.

    3. Hierarchical Zeolites and their Catalytic Performance in Selective Oxidative Processes (pages 1328–1333)

      Dr. Manuel Ojeda, Aida Grau-Atienza, Rafael Campos, Prof. Antonio A. Romero, Dr. Elena Serrano, Prof. Jose Maria Marinas, Prof. Javier García Martínez and Prof. Rafael Luque

      Article first published online: 27 MAR 2015 | DOI: 10.1002/cssc.201500124

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      Ambitious not siliceous: Desilicated hierarchical zeolites hold promise as catalytic systems. The feasibility of using these hierarchical zeolites, with and without iron oxide nanoparticles, in selective oxidation processes is investigated, taking advantage of terminal Al[BOND]OH groups to generate redox sites in zeolites. The test reactions, under microwave irradiation, are the oxidation of benzyl alcohol to benzaldehyde, the epoxidation of cyclohexene, and the multistep conversion of N,N-dimethyl formamide (DMF).

  9. Full Papers

    1. Top of page
    2. Cover Pictures
    3. Cover Profile
    4. Graphical Abstract
    5. Corrigendum
    6. Masthead
    7. News
    8. Minireview
    9. Communications
    10. Full Papers
    1. Mechanism of Brønsted Acid-Catalyzed Glucose Dehydration (pages 1334–1341)

      Dr. Liu Yang, Dr. George Tsilomelekis, Dr. Stavros Caratzoulas and Dr. Dionisios G. Vlachos

      Article first published online: 8 JAN 2015 | DOI: 10.1002/cssc.201403264

      Thumbnail image of graphical abstract

      Glucose dehydration: The DFT-based microkinetic modeling of the Brønsted acid-catalyzed dehydration of glucose is in excellent agreement with experimental kinetic data. The rate-limiting step is the first dehydration of protonated glucose. Isotopic tracing NMR spectroscopy reveals that glucose dehydrates through a cyclic path and the majority of glucose is consumed by the 5-hydroxymethylfurfural intermediate at low conversions.

    2. From Lignocellulosic Biomass to Lactic- and Glycolic-Acid Oligomers: A Gram-Scale Microwave-Assisted Protocol (pages 1342–1349)

      Diego Carnaroglio, Silvia Tabasso, Beata Kwasek, Dariusz Bogdal, Emanuela Calcio Gaudino and Giancarlo Cravotto

      Article first published online: 29 JAN 2015 | DOI: 10.1002/cssc.201403183

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      Not drowning but microwaving: A flash catalytic conversion (2 min) of lignocellulosic biomass into lactic and glycolic acids under microwave irradiation is reported. The batch procedure is successfully adapted to a microwave-assisted flow process, with the aim of designing a scalable process with higher productivity. Good yields and conversions are maintained, productivity is increased and energy consumption is low.

    3. Silver Phosphate/Graphitic Carbon Nitride as an Efficient Photocatalytic Tandem System for Oxygen Evolution (pages 1350–1358)

      Dr. Xiaofei Yang, Dr. Hua Tang, Dr. Jingsan Xu, Prof. Markus Antonietti and Dr. Menny Shalom

      Article first published online: 18 FEB 2015 | DOI: 10.1002/cssc.201403168

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      Composite drawing: Well-defined g-C3N4/Ag3PO4 composite materials are fabricated by using electrostatically driven assembly and ion-exchange processes. Clear evidence for the formation of a Z-scheme between the g-C3N4/Ag3PO4 photocatalyst with outstanding efficiency in oxygen evolution and pollutant degradation is presented. The composite material is superior in both efficiency and stability than pristine Ag3PO4 and C3N4 materials.

    4. Enhancing the Performance of a Robust Sol–Gel-Processed p-Type Delafossite CuFeO2 Photocathode for Solar Water Reduction (pages 1359–1367)

      Mathieu S. Prévot, Dr. Néstor Guijarro and Prof. Kevin Sivula

      Article first published online: 8 JAN 2015 | DOI: 10.1002/cssc.201403146

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      Make the cut: Inexpensive and facile processing aid optimization and allow for insights into the limitations of delafossite CuFeO2, which is a promising material for photoelectrochemical energy conversion. A sol–gel-based technique to prepare thin films of p-type delafossite CuFeO2 on fluorine-doped tin oxide (FTO) glass is described.

    5. Boosting Properties of 3D Binder-Free Manganese Oxide Anodes by Preformation of a Solid Electrolyte Interphase (pages 1368–1380)

      Dr. Haitao Zhou, Xuehang Wang, Dr. Edel Sheridan and Prof. De Chen

      Article first published online: 11 MAR 2015 | DOI: 10.1002/cssc.201403393

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      Full on: A complete solid electrolyte interphase layer is preformed on a pristine 3 D binder-free MnOy-based electrode using a new electrolytic cell, which results in a big boost in the specific energy and cycling stability for the MnOy/LiMn2O4 full cells.

    6. Nanocomposite Membranes based on Polybenzimidazole and ZrO2 for High-Temperature Proton Exchange Membrane Fuel Cells (pages 1381–1393)

      Dr. Graeme Nawn, Dr. Giuseppe Pace, Dr. Sandra Lavina, Dr. Keti Vezzù, Dr. Enrico Negro, Dr. Federico Bertasi, Prof. Stefano Polizzi and Prof. Vito Di Noto

      Article first published online: 20 MAR 2015 | DOI: 10.1002/cssc.201403049

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      The new star in the fuel cell: The development of thermally stable polymer exchange membranes that demonstrate conductivity under anhydrous conditions remains a significant goal for fuel cell technology. This paper describes the structure–property relationships of composite membranes consisting of poly[2,2′-(m-phenylene)-5,5′-bibenzimidazole] impregnated with a ZrO2 nanofiller that has a high ionic conductivity at 185 °C.

    7. Electrosynthesis of Highly Transparent Cobalt Oxide Water Oxidation Catalyst Films from Cobalt Aminopolycarboxylate Complexes (pages 1394–1403)

      Shannon A. Bonke, Dr. Mathias Wiechen, Dr. Rosalie K. Hocking, Dr. Xi-Ya Fang, Prof. Dr. David W. Lupton, Prof. Dr. Douglas R. MacFarlane and Prof. Dr. Leone Spiccia

      Article first published online: 31 MAR 2015 | DOI: 10.1002/cssc.201403188

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      Cover up! Thin, transparent cobalt oxide films, prepared from cobalt polyaminocarboxylate precursors, are shown to be excellent water oxidation catalysts with catalytic activities comparable to those of thicker films derived from Co2+.

    8. Mesoporous Carbon Nitride-Tungsten Oxide Composites for Enhanced Photocatalytic Hydrogen Evolution (pages 1404–1410)

      Dr. Kamalakannan Kailasam, Prof. Dr. Anna Fischer, Guigang Zhang, Dr. Jinshui Zhang, Dr. Michael Schwarze, Marc Schröder, Prof. Dr. Xinchen Wang, Prof. Dr. Reinhard Schomäcker and Prof. Dr. Arne Thomas

      Article first published online: 20 MAR 2015 | DOI: 10.1002/cssc.201403278

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      CN/WO3 composites for enhanced H2 evolution: Mesoporous CN/WO3 composites prepared by a simple dispersion method are efficient photocatalysts for enhanced hydrogen production from water. Compared to other nonporous composites based on carbon nitrides, a twofold increase in activity is observed, which is attributed to the high surface area and efficient solid-state Z-scheme-induced charge separation in these composites.

    9. Conversion of Hemicellulose Sugars Catalyzed by Formic Acid: Kinetics of the Dehydration of D-Xylose, L-Arabinose, and D-Glucose (pages 1411–1428)

      Dr. Karla Dussan, Dr. Buana Girisuta, Marystela Lopes, Dr. James J. Leahy and Prof. Michael H. B. Hayes

      Article first published online: 27 MAR 2015 | DOI: 10.1002/cssc.201403328

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      Hemicellulose's next top model: The pretreatment of lignocellulosic biomass produces liquid streams with hemicellulose sugars, which can be further converted to high-value chemicals. This study investigates the reaction kinetics of the conversion of major hemicellulose sugars of biomass using formic acid as catalyst. Kinetic models are used to model the conversion of sugars in solutions obtained from the fractionation of biomass.

    10. Nanoporous Ru as a Carbon- and Binder-Free Cathode for Li–O2 Batteries (pages 1429–1434)

      Dr. Kaiming Liao, Dr. Tao Zhang, Dr. Yongqing Wang, Dr. Fujun Li, Dr. Zelang Jian, Dr. Haijun Yu and Prof. Haoshen Zhou

      Article first published online: 25 MAR 2015 | DOI: 10.1002/cssc.201403371

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      Reliable ruthenium: A simple method to fabricate nanoporous Ru catalyst for Li–O2 batteries is explored. As a carbon- and binder-free cathode, the nanoporous Ru can be continuously discharged and charged for 100 cycles within a very narrow terminal voltage window and delivers a limited capacity. This good performance is due to strong adhesion of the Ru with the Ni current collector, and good permeation of O2 and electrolyte in the catalyst.

    11. Porous Co3O4/CuO Composite Assembled from Nanosheets as High-Performance Anodes for Lithium-Ion Batteries (pages 1435–1441)

      Qin Hao, Dianyun Zhao, Huimei Duan and Caixia Xu

      Article first published online: 31 MAR 2015 | DOI: 10.1002/cssc.201403420

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      Between the sheets: A porous Co3O4/CuO composite assembled from nanosheets is directly prepared by etching a CoCuAl alloy in NaOH solution. The composite material performs excellently in terms of cycle reversibility, Coulombic efficiency, and rate capability, at both low or high current rates. With the advantages of unique performance and ease of preparation, the as-made Co3O4/CuO nanocomposite demonstrates promising application potential as an advanced anode material for lithium-ion batteries.

    12. Amine-Free Reversible Hydrogen Storage in Formate Salts Catalyzed by Ruthenium Pincer Complex without pH Control or Solvent Change (pages 1442–1451)

      Jotheeswari Kothandaraman, Dr. Miklos Czaun, Dr. Alain Goeppert, Prof. Dr. Ralf Haiges, John-Paul Jones, Robert B. May, Prof. Dr. G. K. Surya Prakash and Prof. Dr. George A. Olah

      Article first published online: 30 MAR 2015 | DOI: 10.1002/cssc.201403458

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      Carbon-neutral cycle! A practical, reversible, and amine-free hydrogen-storage system using Ru-pincer catalyst is presented here. At high H2 pressure, hydrogen combined with CO2 (HCO3) is stored in the form of formate salts. At low pressure, H2 is released. Up to six hydrogenation–dehydrogenation cycles were performed and the catalyst performance remained steady with high selectivity.

    13. Tailoring the Properties of Ammine Metal Borohydrides for Solid-State Hydrogen Storage (pages 1452–1463)

      Lars H. Jepsen, Dr. Morten B. Ley, Prof. Yaroslav Filinchuk, Prof. Flemming Besenbacher and Prof. Torben R. Jensen

      Article first published online: 27 MAR 2015 | DOI: 10.1002/cssc.201500029

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      Here′s my hydride, so tailor me: A series of new ammine metal borohydrides for solid-state hydrogen storage is synthesized, and the crystal structures are solved. The NH3/BH4 ratio for Mn(BH4)2nNH3 is tailored by mechanochemical treatment of the mixture Mn(BH4)2⋅6NH3-Mn(BH4)2 in different ratios. It is shown that for NH3/BH4≤1 hydrogen is released, while ammonia is released for NH3/BH4>1.

    14. Water-Soluble MoS3 Nanoparticles for Photocatalytic H2 Evolution (pages 1464–1471)

      Wei Zhang, Tianhua Zhou, Jianwei Zheng, Jindui Hong, Yunxiang Pan and Prof. Rong Xu

      Article first published online: 31 MAR 2015 | DOI: 10.1002/cssc.201500067

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      Green light for H2 evolution: MoS3 nanoparticles with unusually high water solubility were synthesized through a facile hydrothermal method. Their excellent quantum efficiency for H2 evolution under green light irradiation can be attributed to their good dispersion in water, amorphous nature, abundant surface active sites, higher conduction band potential for proton reduction, and larger indirect band gap for a longer lifetime of the excited electrons.

    15. A Semi-Interpenetrating Network Approach for Dimensionally Stabilizing Highly-Charged Anion Exchange Membranes for Alkaline Fuel Cells (pages 1472–1483)

      Steve S. He, Alaina L. Strickler and Prof. Curtis W. Frank

      Article first published online: 27 MAR 2015 | DOI: 10.1002/cssc.201500133

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      A little restraint can work wonders: Increasing the ion exchange capacity of an anion exchange membrane often leads to higher conductivity at the expense of excessive swelling and decreased mechanical stability. We employ a semi-interpenetrating network architecture to dimensionally stabilize highly-charged benzyltrimethylammonium polysulfone membranes. These reinforced membranes exhibit excellent ionic conductivity and mechanical robustness.

    16. Superior Lithium Storage Performance using Sequentially Stacked MnO2/Reduced Graphene Oxide Composite Electrodes (pages 1484–1491)

      Sue Jin Kim, Young Jun Yun, Ki Woong Kim, Changju Chae, Dr. Sunho Jeong, Dr. Yongku Kang, Dr. Si-Young Choi, Dr. Sun Sook Lee and Dr. Sungho Choi

      Article first published online: 2 APR 2015 | DOI: 10.1002/cssc.201500200

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      Perfecting the filling: A facile synthesis of sandwich-like stacked “α-MnO2 nanowire/reduced graphene oxide sheets” composite electrodes are reported for superior lithium ion rechargeable battery. A synergistic effect of multidimensional nanoscale media between one (metal oxide nanowire) and two dimensions (graphene sheet) is observed.

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