ChemSusChem

Cover image for Vol. 6 Issue 5

May 2013

Volume 6, Issue 5

Pages 731–927

  1. Cover Picture

    1. Top of page
    2. Cover Picture
    3. Cover Profile
    4. Graphical Abstract
    5. Masthead
    6. News
    7. Review
    8. Highlight
    9. Communications
    10. Full Papers
    1. You have free access to this content
      Cover Picture: Oxygen-Functionalized Few-Layer Graphene Sheets as Active Catalysts for Oxidative Dehydrogenation Reactions (ChemSusChem 5/2013) (page 731)

      Dr. Viviane Schwartz, Dr. Wujun Fu, Dr. Yu-Tung Tsai, Dr. Harry M. Meyer III, Dr. Adam J. Rondinone, Jihua Chen, Dr. Zili Wu, Dr. Steven H. Overbury and Dr. Chengdu Liang

      Version of Record online: 2 MAY 2013 | DOI: 10.1002/cssc.201390019

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      The cover picture shows an illustration of a graphene sheet decorated with different types of oxygen functionalities and the oxidative dehydrogenation reaction of isobutane to isobutene that is catalyzed by the functionalized edge sites. The micrograph background image is of the same graphenes recorded by Schwartz et al using a new helium-ion microscope at the Center for Nanophase Materials Sciences/Oak Ridge National Laboratory (CNMS/ORNL). The application of oxygen-modified graphene for gas-phase reactions, which is reported on page 840, is a new approach to study the scarcely explored field of carbon catalysis. This field of metal-free carbon-based catalysis is of importance for developing a more sustainable and environmentally friendly catalytic oxidative dehydrogenation process as carbon materials can be easily disposed of after their lifetime.

  2. Cover Profile

    1. Top of page
    2. Cover Picture
    3. Cover Profile
    4. Graphical Abstract
    5. Masthead
    6. News
    7. Review
    8. Highlight
    9. Communications
    10. Full Papers
    1. You have free access to this content
      Oxygen-Functionalized Few-Layer Graphene Sheets as Active Catalysts for Oxidative Dehydrogenation Reactions (page 732)

      Dr. Viviane Schwartz, Dr. Wujun Fu, Dr. Yu-Tung Tsai, Dr. Harry M. Meyer III, Dr. Adam J. Rondinone, Jihua Chen, Dr. Zili Wu, Dr. Steven H. Overbury and Dr. Chengdu Liang

      Version of Record online: 2 MAY 2013 | DOI: 10.1002/cssc.201300357

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      Invited for this months cover is the group from the Center for Nanophase Materials Sciences (CNMS) at the Oak Ridge National Laboratory. The illustration is of the catalytic activity of the reported oxygen-functionalized few-layer graphenes, whereas the micrograph background image is of the same graphenes recorded by the authors using a new helium-ion microscope at the CNMS. Read the full text of the article at 10.1002/cssc.201200756

  3. Graphical Abstract

    1. Top of page
    2. Cover Picture
    3. Cover Profile
    4. Graphical Abstract
    5. Masthead
    6. News
    7. Review
    8. Highlight
    9. Communications
    10. Full Papers
    1. You have free access to this content
  4. Masthead

    1. Top of page
    2. Cover Picture
    3. Cover Profile
    4. Graphical Abstract
    5. Masthead
    6. News
    7. Review
    8. Highlight
    9. Communications
    10. Full Papers
    1. Masthead: ChemSusChem 5/2013 (page 741)

      Version of Record online: 2 MAY 2013 | DOI: 10.1002/cssc.201390021

  5. News

    1. Top of page
    2. Cover Picture
    3. Cover Profile
    4. Graphical Abstract
    5. Masthead
    6. News
    7. Review
    8. Highlight
    9. Communications
    10. Full Papers
  6. Review

    1. Top of page
    2. Cover Picture
    3. Cover Profile
    4. Graphical Abstract
    5. Masthead
    6. News
    7. Review
    8. Highlight
    9. Communications
    10. Full Papers
    1. Novel Process Windows for Enabling, Accelerating, and Uplifting Flow Chemistry (pages 746–789)

      Prof. Dr. Volker Hessel, Dr. Dana Kralisch, Prof. Dr. Norbert Kockmann, Dr. Timothy Noël and Dr. Qi Wang

      Version of Record online: 18 APR 2013 | DOI: 10.1002/cssc.201200766

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      Windows provide panoramas: Novel Process Windows are a chance to explore new horizons for the processing industry. They make use of process conditions that are far from conventional practices. This Review discusses different routes and provides several examples for each route based on chemical and process-design intensification classification (see picture).

  7. Highlight

    1. Top of page
    2. Cover Picture
    3. Cover Profile
    4. Graphical Abstract
    5. Masthead
    6. News
    7. Review
    8. Highlight
    9. Communications
    10. Full Papers
    1. A Noble-Metal-Free System for Photodriven Catalytic Proton Reduction (pages 790–793)

      Bart van den Bosch, Hung-Cheng Chen, Dr. Jarl Ivar van der Vlugt, Prof. Dr. Albert M. Brouwer and Prof. Dr. Joost N. H. Reek

      Version of Record online: 19 MAR 2013 | DOI: 10.1002/cssc.201200960

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      Who needs the nobles? Ideally, devices to harvest solar energy into fuels would, in addition to having very high turnover numbers, make use of earth-abundant materials. In this Highlight we focus on a recent example in which a copper-based photosensitizer is used, in combination with an iron-based catalyst for light-driven proton reduction.

  8. Communications

    1. Top of page
    2. Cover Picture
    3. Cover Profile
    4. Graphical Abstract
    5. Masthead
    6. News
    7. Review
    8. Highlight
    9. Communications
    10. Full Papers
    1. Organic Rechargeable Batteries with Tailored Voltage and Cycle Performance (pages 794–797)

      Dr. Shinsuke Nishida, Yosuke Yamamoto, Prof. Dr. Takeji Takui and Prof. Dr. Yasushi Morita

      Version of Record online: 15 MAR 2013 | DOI: 10.1002/cssc.201300010

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      Made to order: Rechargeable batteries are fabricated by using organic electron acceptors and donors as active cathode materials. Their output voltage and cycle performance can be tuned by organic chemistry techniques. The output voltages are linked to both the redox potentials and the energy levels of the frontier molecular orbitals of the cathode materials, enabling to predict the output voltage at an early stage of the design.

    2. Selective Hydrodeoxygenation of Biomass-Derived Oxygenates to Unsaturated Hydrocarbons using Molybdenum Carbide Catalysts (pages 798–801)

      Hui Ren, Weiting Yu, Michael Salciccioli, Ying Chen, Yulin Huang, Ke Xiong, Prof. Dionisios G. Vlachos and Prof. Jingguang G. Chen

      Version of Record online: 4 APR 2013 | DOI: 10.1002/cssc.201200991

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      Which cleavage do you prefer? With a combination of density functional theory (DFT) calculations, surface science studies, and reactor evaluations, Mo2C is identified as a highly selective HDO catalyst to selectively convert biomass-derived oxygenates to unsaturated hydrocarbons through selective C[BOND]O bond scissions without C[BOND]C bond cleavage. This provides high-value HDO products for utilization as feedstocks for chemicals and fuels; this also reduces the overall consumption of H2.

    3. A Solar Rechargeable Flow Battery Based on Photoregeneration of Two Soluble Redox Couples (pages 802–806)

      Ping Liu, Yu-liang Cao, Guo-Ran Li, Xue-Ping Gao, Xin-Ping Ai and Prof. Han-Xi Yang

      Version of Record online: 4 APR 2013 | DOI: 10.1002/cssc.201200962

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      Storable sunshine, reusable rays: A solar rechargeable redox flow battery is proposed based on the photoregeneration of I3/I and [Fe(C10H15)2]+/Fe(C10H15)2 soluble redox couples, which can be regenerated by flowing from a discharged redox flow battery (RFB) into a dye-sensitized solar cell (DSSC) and then stored in tanks for subsequent RFB applications This technology enables effective solar-to-chemical energy conversion.

    4. Nitrogen-Enriched Carbon from Melamine Resins with Superior Oxygen Reduction Reaction Activity (pages 807–812)

      Dr. Hexiang Zhong, Prof. Huamin Zhang, Sisi Liu, Chengwei Deng and Meiri Wang

      Version of Record online: 11 MAR 2013 | DOI: 10.1002/cssc.201200919

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      Catalytic carbon: Nitrogen-doped porous carbon (CNx) electrocatalysts are derived from inexpensive melamine formaldehyde resins. These potential PEMFC catalysts are synthesized by using a facile method, which yields materials that contain a meso- and macroporous structure. The carbon-based materials display attractive catalytic activity toward ORR and superior stability compared to a commercial Pt-based catalyst.

    5. From Hazardous Waste to Valuable Raw Material: Hydrolysis of CCA-treated Wood for the Production of Chemicals (pages 813–815)

      Maija Hakola, Anne Kallioinen, Prof. Markku Leskelä and Prof. Timo Repo

      Version of Record online: 3 APR 2013 | DOI: 10.1002/cssc.201200754

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      Solid wood, metal finnish: Instead of burning waste wood treated with chromated copper arsenite (CCA) or disposing of it in landfills, the CCA-treated wood can be used as a raw material for the production of chemicals. Catalytic or alkaline oxidation together with very mild sulfuric acid extraction produces an easily enzymatically hydrolyzable material. Usage as a raw material for the chemical industry in this manner demonstrates a sustainable and value-added waste management process.

    6. Hydrogen Production by Dehydrogenation of Formic Acid on Atomically Dispersed Gold on Ceria (pages 816–819)

      Nan Yi, Prof. Howard Saltsburg and Prof. Maria Flytzani-Stephanopoulos

      Version of Record online: 26 MAR 2013 | DOI: 10.1002/cssc.201200957

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      Less is More: Atomically dispersed gold species catalyze the decomposition of formic acid through the dehydrogenation pathway at near-ambient temperatures. Gold on ceria is demonstrated to be an effective and stable catalyst. By using this catalyst, mechanistic insights are obtained that can lead to the use of trace amounts of gold to achieve robust and cost-effective catalysts.

  9. Full Papers

    1. Top of page
    2. Cover Picture
    3. Cover Profile
    4. Graphical Abstract
    5. Masthead
    6. News
    7. Review
    8. Highlight
    9. Communications
    10. Full Papers
    1. Catalytic Dehydration of Carbohydrates on In Situ Exfoliatable Layered Niobic Acid in an Aqueous System under Microwave Irradiation (pages 820–825)

      Qingbin Wu, Yani Yan, Qian Zhang, Jinhua Lu, Zhijian Yang, Prof. Yahong Zhang and Prof. Yi Tang

      Version of Record online: 18 APR 2013 | DOI: 10.1002/cssc.201300004

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      Between the sheets: A simple and efficient microwave-assisted HNb3O8 catalytic process is proposed for the dehydration of carbohydrates in a sustainable pure aqueous system, in which the fast in situ exfoliation of the layered HNb3O8 under microwave irradiation is crucial for the remarkable catalytic performance.

    2. Lipase-Mediated Selective Oxidation of Furfural and 5-Hydroxymethylfurfural (pages 826–830)

      Monika Krystof, Dr. María Pérez-Sánchez and Dr. Pablo Domínguez de María

      Version of Record online: 10 APR 2013 | DOI: 10.1002/cssc.201200954

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      Value added per-acid: The use of lipases as biocatalysts for the in situ production of organic peracids has been explored. A new peracid-based methodology for the oxidative valorization of biomass-derived furanics is subsequently formulated. This may bring innovative approaches in the field once optimization and process-development considerations are taken into account.

    3. Highly Selective Lewis Acid Sites in Desilicated MFI Zeolites for Dihydroxyacetone Isomerization to Lactic Acid (pages 831–839)

      Pierre Y. Dapsens, Dr. Cecilia Mondelli and Prof. Javier Pérez-Ramírez

      Version of Record online: 3 APR 2013 | DOI: 10.1002/cssc.201200703

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      Making the right site: Lewis acid centers generated upon the desilication of commercial MFI zeolites in alkaline media are shown to catalyze the isomerization of dihydroxyacetone to lactic acid, competing with tin-containing zeolites. This opens exciting perspectives for the use of hierarchical zeolites with tailored porous and acidic properties in biomass-to-chemical conversions.

    4. Oxygen-Functionalized Few-Layer Graphene Sheets as Active Catalysts for Oxidative Dehydrogenation Reactions (pages 840–846)

      Dr. Viviane Schwartz, Dr. Wujun Fu, Dr. Yu-Tung Tsai, Dr. Harry M. Meyer III, Dr. Adam J. Rondinone, Jihua Chen, Dr. Zili Wu, Dr. Steven H. Overbury and Dr. Chengdu Liang

      Version of Record online: 7 MAR 2013 | DOI: 10.1002/cssc.201200756

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      Edge exposure: Few-layer graphene and its oxygen-functionalized form are used to investigate the nature of graphitic active sites for the heterogeneous catalytic oxidative dehydrogenation reaction. No clear correlation is observed between isobutane consumption rate and the oxygen content of the samples; therefore, demonstrating that not all of the oxygen functionalities are active for this reaction.

    5. Platinum- and Membrane-Free Swiss-Roll Mixed-Reactant Alkaline Fuel Cell (pages 847–855)

      Amin Aziznia, Colin W. Oloman and Előd L. Gyenge

      Version of Record online: 15 APR 2013 | DOI: 10.1002/cssc.201300127

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      Roll with it: A mixed-reactant alkaline borohydride–oxygen fuel cell with a Swiss-roll design is presented, which uses an osmium anode and a manganese dioxide gas-diffusion cathode. For a single-cell mixed-reactant fuel cell, a superficial peak power density of 1880 W m−2 is achieved, which is higher than any low temperature mixed-reactant fuel cell so far reported in the literature with an anode electrocatalyst loading of less than 0.5 mg cm−2.

    6. Bragg Stack-Functionalized Counter Electrode for Solid-State Dye-Sensitized Solar Cells (pages 856–864)

      Dr. Jung Tae Park, Jacob H. Prosser, Dong Jun Kim, Prof. Jong Hak Kim and Prof. Daeyeon Lee

      Version of Record online: 9 APR 2013 | DOI: 10.1002/cssc.201300117

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      What′s in your reflection? A highly reflective counter electrode based on a Bragg stack is prepared by the deposition of alternating layers of organized mesoporous TiO2 and colloidal SiO2 nanoparticles. By using this in conjunction with a polymerized ionic liquid, the energy conversion efficiency of the solid-state dye-sensitized solar cell (ssDSSC) is among the highest of ssDSSCs based on the N719 dye.

    7. Superior Performance of Metal–Organic Frameworks over Zeolites as Solid Acid Catalysts in the Prins Reaction: Green Synthesis of Nopol (pages 865–871)

      Dr. Maksym Opanasenko, Dr. Amarajothi Dhakshinamoorthy, Dr. Young Kyu Hwang, Dr. Jong-San Chang, Prof. Hermenegildo Garcia and Prof. Jiří Čejka

      Version of Record online: 16 APR 2013 | DOI: 10.1002/cssc.201300032

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      Green and efficient: Its high activity in the Prins condensation of β-pinene and paraformaldehyde, the preservation of its structure and active sites, and the possibility to use MIL-100 (Fe) in at least three catalytic cycles without loss of its activity are established. Our report exemplifies the advantages of MOFs over zeolites as solid catalysts in liquid-phase reactions for the production of fine chemicals.

    8. A Comprehensive Study on the Activity and Deactivation of Immobilized Lecitase Ultra in Esterifications of Food Waste Streams to Monoacylglycerols (pages 872–879)

      Karen M. Gonçalves, Felipe K. Sutili, Ivaldo I. Júnior, Marcella C. Flores, Dr. Leandro Soter de Mariz e Miranda, Dr. Ivana C. R. Leal, Dr. Yraima Cordeiro, Dr. Rafael Luque and Dr. Rodrigo Octavio M. Alves de Souza

      Version of Record online: 19 MAR 2013 | DOI: 10.1002/cssc.201300026

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      Trapped into action: Lecitase Ultra is immobilized on Amberlites XAD2 and XAD4 through physical entrapping under conventional stirring or ultrasound irradiation (see picture). The resulting immobilized biocatalysts are utilized in the valorization of an acidic food-derived residue from a palm oil refining process to produce monoacylglycerols from isopropylidene glycerol under batch and continuous flow conditions.

    9. Porous Graphitic Carbon Nanosheets Derived from Cornstalk Biomass for Advanced Supercapacitors (pages 880–889)

      Dr. Lei Wang, Dr. Guang Mu, Dr. Chungui Tian, Dr. Li Sun, Dr. Wei Zhou, Peng Yu, Jie Yin and Prof. Honggang Fu

      Version of Record online: 18 APR 2013 | DOI: 10.1002/cssc.201200990

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      Fields of gold? Porous graphitic carbon nanosheets (PGCS) have been synthesized by a self-generating template strategy based on the carburized effect of iron with cornstalks. The synthesized PGCS exhibit excellent capacitive performance owing to their unique porous nanostructures and graphitic carbon nanosheets, which can facilitate ion and electron transport, respectively.

    10. Carboxylate-Assisted Formation of Alkylcarbonate Species from CO2 and Tetramethylammonium Salts with a β-Amino Acid Anion (pages 890–897)

      Sung Yun Hong, Youngeun Cheon, Seung Hoon Shin, Dr. Hyunjoo Lee, Dr. Minserk Cheong and Dr. Hoon Sik Kim

      Version of Record online: 9 APR 2013 | DOI: 10.1002/cssc.201200971

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      Catch me if you can: Tetramethylammonium salts bearing a β-amino acid anion (TMAAs) are synthesized through Michael addition reactions of amines with methyl acrylate, subsequent hydrolysis, and neutralization with aqueous tetramethylammonium hydroxide. These TMAAs interact with CO2 in a 1:1 mode in ethylene glycol, which forms hydroxyethylcarbonate species. The driving force for the 1:1 bonding appears to be the intramolecular hydrogen bonding network exerted through the carboxylate group.

    11. Reduced Graphite Oxide/Nano Sn: A Superior Composite Anode Material for Rechargeable Lithium-Ion Batteries (pages 898–904)

      Dr.  Chandrasekaran Nithya and Dr.  Sukumaran Gopukumar

      Version of Record online: 19 MAR 2013 | DOI: 10.1002/cssc.201200970

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      RGO/Nano Sn: This study investigates the electrochemical performance of reduced graphite oxide (RGO) anchored with nano Sn. This material demonstrates superior electrochemical performance that is associated with the flexible RGO matrix and the uniform distribution of Sn particles, which reduce the lithium-ion diffusion path length; therefore, the RGO matrix provides more stability to tin particles during cycling.

    12. Chemoselective CaO-Mediated Acylation of Alcohols and Amines in 2-Methyltetrahydrofuran (pages 905–910)

      Dr. Vittorio Pace, Dr. Pilar Hoyos, Prof. Dr. Andrés R. Alcántara and Prof. Dr. Wolfgang Holzer

      Version of Record online: 26 MAR 2013 | DOI: 10.1002/cssc.201200922

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      Scrounger! A sustainable chemoselective protocol is presented for the stoichiometric acylation of alcohols and amines. This methodology utilises CaO as an effective acid scavenger. Acylation of primary alcohols is achieved chemoselectively over phenols or tertiary alcohols. Improved yields are obtained by using biocompatible 2-methyltetrahydrofuan instead of diethyl ether.

    13. Synthesis of DNL-6 with a High Concentration of Si (4 Al) Environments and its Application in CO2 Separation (pages 911–918)

      Xiong Su, Dr. Peng Tian, Dong Fan, Prof. Qinghua Xia, Yue Yang, Dr. Shutao Xu, Dr. Lin Zhang, Dr. Ying Zhang, Dehua Wang and Prof. Zhongmin Liu

      Version of Record online: 18 APR 2013 | DOI: 10.1002/cssc.201200907

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      Supplementary Si, superior selectivity: DNL-6, which is an isomorphous crystal of the RHO zeolite with a silicoaluminophosphate (SAPO) composition, is synthesized with a high concentration of Si (4 Al) environments (M-DNL-6). This zeolite demonstrates efficient CO2 adsorption and is shown to effectively separate CO2 from CH4 and N2. It is also shown that M-DNL-6 can be regenerated under very mild conditions.

    14. pH-Induced Lignin Surface Modification to Reduce Nonspecific Cellulase Binding and Enhance Enzymatic Saccharification of Lignocelluloses (pages 919–927)

      Prof. Hongming Lou, Prof. J. Y. Zhu, Tian Qing Lan, Huanran Lai and Prof. Xueqing Qiu

      Version of Record online: 28 MAR 2013 | DOI: 10.1002/cssc.201200859

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      Phenomenon: We investigate the mechanism of the significant enhancement in the enzymatic saccharification of lignocelluloses at an elevated pH of 5.5–6.0. An elevated pH significantly increases the lignin surface charge, which causes lignin to become more hydrophilic and facilitates the electrostatic interactions between cellulose and lignin to reduce its coordination affinity to cellulase and, consequently, the nonspecific binding of cellulase.

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