ChemSusChem

Cover image for Vol. 6 Issue 1

January 2013

Volume 6, Issue 1

Pages 1–208

  1. Cover Picture

    1. Top of page
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    3. Cover Profile
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    5. Editorial
    6. Masthead
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    10. Review
    11. Minireview
    12. Communications
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      Cover Picture: The Effect of Switchable Water Additives on Clay Settling (ChemSusChem 1/2013) (page 1)

      Chien-Shun Chen, Ying Yin Lau, Sean M. Mercer, Dr. Tobias Robert, Prof. Dr. J. Hugh Horton and Prof. Dr. Philip G. Jessop

      Article first published online: 11 JAN 2013 | DOI: 10.1002/cssc.201390000

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      The cover picture illustrates the use of switchable water, an aqueous solution with a CO2-switchable ionic strength, to expedite the settling of clay solids without making the process water permanently salty. In strip mining operations, the settling of fine solids such as clay particles from aqueous suspensions is often a time- and material-intensive process. In their Full paper on page 132, Horton and Jessop describe how calcium salts can be used to promote the settling of the solids; however, the liberated salts must then be desalinated before recycling. Using switchable water, the introduction of CO2 increases the ionic strength of the aqueous solution by reacting with an amine additive, thus promoting clay settling. The later removal of CO2 from the liberated water decreases the ionic strength, allowing the water to be recycled.

  2. Cover Profile

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      The Effect of Switchable Water Additives on Clay Settling (page 2)

      Article first published online: 11 JAN 2013 | DOI: 10.1002/cssc.201200932

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      “If one had an easy way to decontaminate water, a method that allows the water to be recycled without expensive purification steps, then water might really live up to its green potential.” This and more about the story behind the front cover research can be found on p. 2.

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      Back Cover: Conversion of (Ligno)Cellulose Feeds to Isosorbide with Heteropoly Acids and Ru on Carbon (ChemSusChem 1/2013) (page 209)

      Beau Op de Beeck, Dr. Jan Geboers, Dr. Stijn Van de Vyver, Jonas Van Lishout, Jeroen Snelders, Dr. Wouter J. J. Huijgen, Prof. Dr. Christophe M. Courtin, Prof. Dr. Pierre A. Jacobs and Prof. Dr. Bert F. Sels

      Article first published online: 11 JAN 2013 | DOI: 10.1002/cssc.201390005

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      The back cover picture shows the sequential steps for the conversion of wheat straw to isosorbide: organosolv pretreatment of wheat straw to delignified pulp followed by one-pot hydrolytic hydrogenation and dehydration to isosorbide with heteropoly acids and Ru/C, as described by Sels et al. on page 199. The carbon cycle is tentatively closed via CO2 uptake from the end products (e.g. polymers, surfactants) by the wheat plants.

  4. Editorial

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      Editorial: All Signals Green for ChemSusChem (pages 3–5)

      Guido M. Kemeling

      Article first published online: 11 JAN 2013 | DOI: 10.1002/cssc.201200948

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      In this Editorial we look back on 2012 and forward to what 2013 has to offer. ChemSusChem grew very strongly in 2012, and a number of topical issues further defined the journal′s scope. From 2013 onwards, Licheng Sun will take the reigns as one of our three Chairmen, while we introduce new features aimed at making the journal more attractive. Outside of ChemSusChem, the Smart Article debuts at Chemistry–An Asian Journal while Angewandte Chemie celebrates the publication of its 125th volume!

  5. Masthead

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    1. Masthead: ChemSusChem 1/2013 (page 6)

      Article first published online: 11 JAN 2013 | DOI: 10.1002/cssc.201390003

  6. Graphical Abstract

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    1. Graphical Abstract: ChemSusChem 1/2013 (pages 7–14)

      Article first published online: 11 JAN 2013 | DOI: 10.1002/cssc.201390004

  7. Masthead

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    1. Masthead: ChemSusChem 1/2013 (page 15)

      Article first published online: 11 JAN 2013 | DOI: 10.1002/cssc.201390001

  8. News

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    1. Spotlights on our sister journals: ChemSusChem 1/2013 (pages 16–19)

      Article first published online: 11 JAN 2013 | DOI: 10.1002/cssc.201390002

  9. Review

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      Materials for the Active Layer of Organic Photovoltaics: Ternary Solar Cell Approach (pages 20–35)

      Dr. Yung-Chung Chen, Dr. Chih-Yu Hsu, Ryan Yeh-Yung Lin, Prof. Kuo-Chuan Ho and Prof. Jiann T. Lin

      Article first published online: 3 JAN 2013 | DOI: 10.1002/cssc.201200609

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      All good things come in threes: Addition of a third component in bulk heterojunction solar cells (sensitizer or fullerene derivative) may increase the short-circuit current through enhanced light harvesting and/or can increase the open-circuit voltage through enhanced carrier mobility and modification of HOMO/LUMO energy levels. Such ternary organic solar cell systems will be reviewed in this article.

  10. Minireview

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    1. Harmonising Production, Properties and Environmental Consequences of Liquid Transport Fuels from Biomass—2,5-Dimethylfuran as a Case Study (pages 36–41)

      Prof. John M. Simmie and Dr. Judith Würmel

      Article first published online: 17 DEC 2012 | DOI: 10.1002/cssc.201200738

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      Fuel for the future? 2,5-Dimethylfuran has been the subject of many recent studies since its potential as a ‘green next-generation’ biofuel was highlighted in 2007. The chemistry of this compound is characterised by unusually strong ring-carbon-to-hydrogen bonds, and some of its derivatives are distinguished by extremely weak bonds. This combination makes the task of unravelling their chemistry, and the impacts on the environment and human health, both interesting and challenging.

  11. Communications

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      A Versatile Aqueous Reduction of Bio-Based Carboxylic Acids using Syngas as a Hydrogen Source (pages 42–46)

      Lei Yu, Dr. Xian-Long Du, Jing Yuan, Dr. Yong-Mei Liu, Prof. Dr. Yong Cao, He-Yong He and Prof. Kang-Nian Fan

      Article first published online: 9 NOV 2012 | DOI: 10.1002/cssc.201200674

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      Syngas as a versatile hydrogen source: Using readily available and economically favorable syngas as a convenient hydrogen source, an efficient and sustainable aqueous reduction of bio-based carboxylic acids has been achieved over a highly robust catalyst system consisting of gold nanoparticles supported on acid-tolerant single-phase monoclinic zirconia (Au/m-ZrO2). A range of bio-based multifunctional carboxylic acids have been selectively converted into their corresponding lactones or diols in high to excellent yields.

    2. Catalytic Conversion of Furfural into a 2,5-Furandicarboxylic Acid-Based Polyester with Total Carbon Utilization (pages 47–50)

      Tao Pan, Jin Deng, Qing Xu, Yong Zuo, Prof. Qing-Xiang Guo and Prof. Dr. Yao Fu

      Article first published online: 13 DEC 2012 | DOI: 10.1002/cssc.201200652

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      One divided into two combined into one: The catalytic conversion of furfural into a 2,5-furandicarboxylic acid-based polyester, linked by the disproportionation of furoate to furan and 2,5-furandicarboxylate, is reported. In this manner, all carbons are utilized, demonstrating the success of combining a platform molecule from C5 sugars (furfural) to one from C6 sugars (2,5-FDCA).

    3. The Effect of Oxygen Crossover on the Anode of a Li–O2 Battery using an Ether-Based Solvent: Insights from Experimental and Computational Studies (pages 51–55)

      Dr. Rajeev S. Assary, Dr. Jun Lu, Dr. Peng Du, Xiangyi Luo , Dr. Xiaoyi Zhang, Dr. Yang Ren, Dr. Larry A. Curtiss and Dr. Khalil Amine

      Article first published online: 3 DEC 2012 | DOI: 10.1002/cssc.201200810

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      Crosstown traffic: Further development of Li–O2 batteries may eventually lead to their use in transportation applications. One problem that needs to be addressed is electrolyte decomposition, which has been partially mitigated by using ether- rather than carbonate-based solvents. The influence of oxygen crossover from the cathode to the anode on electrolyte, and lithium anode, decomposition in ether-based Li-O2 batteries is investigated.

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      Nitrogen-Doped Porous Carbon Nanosheets as Low-Cost, High-Performance Anode Material for Sodium-Ion Batteries (pages 56–60)

      Dr. Heng-guo Wang, Zhong Wu , Fan-lu Meng , De-long Ma , Xiao-lei Huang , Prof. Dr. Li-min Wang and Prof. Dr. Xin-bo Zhang

      Article first published online: 7 DEC 2012 | DOI: 10.1002/cssc.201200680

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      Between the sheets: Sodium-ion batteries are an attractive, low-cost alternative to lithium-ion batteries. Nitrogen-doped porous carbon sheets are prepared by chemical activation of polypyrrole-functionalized graphene sheets. When using the sheets as anode material in sodium-ion batteries, their unique compositional and structural features result in high reversible capacity, good cycling stability, and high rate capability.

    5. Chromium(0) Nanoparticles as Effective Catalyst for the Conversion of Glucose into 5-Hydroxymethylfurfural (pages 61–64)

      Dr. Jianghua He, Dr. Yuetao Zhang and Prof. Dr. Eugene Y.-X. Chen

      Article first published online: 7 DEC 2012 | DOI: 10.1002/cssc.201200795

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      It′s nano: Small and uniform chromium nanoparticles, either preformed or generated in situ, effectively catalyze the conversion of glucose into 5-hydroxymethyl furfural. The results compare favorably with those achieved by using a catalyst system based on divalent CrCl2 in ionic liquids (ILs). In addition, the chromium nanoparticles are found in the CrCl2/IL system, and the implications of their presence in that system is investigated.

  12. Full Papers

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    1. Photo-active Cobalt Cubane Model of an Oxygen-Evolving Catalyst (pages 65–69)

      Dr. Mark D. Symes, Dr. Daniel A. Lutterman, Dr. Thomas S. Teets, Bryce L. Anderson, Prof. John J. Breen and Prof. Daniel G. Nocera

      Article first published online: 3 JAN 2013 | DOI: 10.1002/cssc.201200682

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      Down to the core: A soluble molecular model of a cobalt-based oxygen-evolving catalyst has been appended to ReI photosensitizers, giving rise to an unusual coordination complex consisting of an inorganic metal-oxo core tethered to two photo-sensitising oxidants. Substantial emission quenching of the ReI photocentres is evident upon irradiation at 355 nm.

    2. Co-sensitization of Organic Dyes for Efficient Dye-Sensitized Solar Cells (pages 70–77)

      Dr. Ming Cheng, Prof. Xichuan Yang, Dr. Jiajia Li, Dr. Fuguo Zhang and Prof. Licheng Sun

      Article first published online: 27 NOV 2012 | DOI: 10.1002/cssc.201200655

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      Sensitive dyes absorb it all: Co-sensitization of three spectrally complementary dyes on a TiO2 film in a well-designed sequence significantly improves the photovoltaic performance of the device, and an efficiency of 8.2 % is achieved. The devices demonstrate a panchromatic response with an incident photon-to-current conversion efficiency >80 % over the entire visible spectral region from 400 to 700 nm.

    3. Nanoporous PdTi Alloys as Non-Platinum Oxygen-Reduction Reaction Electrocatalysts with Enhanced Activity and Durability (pages 78–84)

      Yunqing Liu and Prof. Caixia Xu

      Article first published online: 23 NOV 2012 | DOI: 10.1002/cssc.201200752

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      Digested metals reduce oxygen: A nanoporous PdTi (NP-PdTi) alloy characterized by a 3D bicontinuous network nanostructure can be easily fabricated by a one-step mild dealloying process of PdTiAl (precursor alloy). With a ligament size as small as 6 nm, NP-PdTi shows superior electrocatalytic activity in the oxygen reduction reaction with enhanced specific and mass activities as well as higher methanol tolerance and structure stability relative to Pt/C.

    4. Synthesis of Stable Phosphomide Ligands and their Use in Ru-Catalyzed Hydrogenations of Bicarbonate and Related Substrates (pages 85–91)

      Dr. Saravanan Gowrisankar, Dr. Christopher Federsel, Dr. Helfried Neumann, Carolin Ziebart, Dr. Ralf Jackstell, Dr. Anke Spannenberg and Prof. Dr. Matthias Beller

      Article first published online: 28 DEC 2012 | DOI: 10.1002/cssc.201200732

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      Ruthenium and phosphor work wonders: Air-stable ruthenium phosphomide complexes are active catalysts in the hydrogenation of sodium bicarbonate, carbon dioxide, and carbonyl compounds. Hydrogenation proceeds with high catalyst turnover numbers in the absence of amines or other additives. The application range of these new ruthenium catalysts also includes the hydrogenation of cinnamaldehyde and benzaldehyde.

    5. Investigation and Enhancement of the Stability and Performance of Water Reduction Systems based on Cyclometalated Iridium(III) Complexes (pages 92–101)

      Sven Hansen, Dr. Marga-Martina Pohl, Dr. Marcus Klahn, Dr. Anke Spannenberg and Dr. Torsten Beweries

      Article first published online: 12 NOV 2012 | DOI: 10.1002/cssc.201200617

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      Teamwork 2.0: A highly active system for photocatalytic water reduction consisting of an Ir photosensitiser and a Pd dichloro complex as the source of catalytically active Pd0 is described. Additionally, the introduction of a hitherto unknown dinuclear Co complex as a water reduction centre resulted in a system with a comparably high initial activity.

    6. Structural and Photoelectrochemical Evaluation of Nanotextured Sn-Doped AgInS2 Films Prepared by Spray Pyrolysis (pages 102–109)

      Qian Cheng, Prof. Xihong Peng and Prof. Candace K. Chan

      Article first published online: 23 DEC 2012 | DOI: 10.1002/cssc.201200588

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      Tin best or tin pest? The role of Sn extrinsic dopants in chalcopyrite AgInS2 is investigated to understand their effects on the optical, electronic, and photoelectrochemical properties of this promising photoanode material. We found that at low amounts, Sn increased the AgInS2 carrier concentration and photocurrent, but was detrimental at higher dopant concentrations.

    7. Optimization of Hydrothermal Pretreatment of Lignocellulosic Biomass in the Bioethanol Production Process (pages 110–122)

      Christos K. Nitsos, Prof. Konstantinos A. Matis and Prof. Kostas S. Triantafyllidis

      Article first published online: 23 NOV 2012 | DOI: 10.1002/cssc.201200546

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      Green fuels and chemicals: The enzymatic digestibility of cellulose in lignocellulosic biomass towards fermentable glucose can be increased significantly by hydrothermal pretreatment in pure water under relatively mild conditions. Appropriate selection of the pretreatment temperature and time also leads to a process liquid that can be enriched in xylose or in furfural and acetic acid.

    8. From Biomass to Chemicals: Synthesis of Precursors of Biodegradable Surfactants from 5-Hydroxymethylfurfural (pages 123–131)

      K. S. Arias, Saud I. Al-Resayes, Maria J. Climent, Avelino Corma and Sara Iborra

      Article first published online: 9 JAN 2013 | DOI: 10.1002/cssc.201200513

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      From HMF to surfactants: Precursors of surfactant molecules are obtained by a two-step one-pot selective acetalization and transacetalization of 5-hydroxymethylfurfural with long-chain alkyl alcohols by controlling the zeolite acidity and polarity.

    9. The Effect of Switchable Water Additives on Clay Settling (pages 132–140)

      Chien-Shun Chen, Ying Yin Lau, Sean M. Mercer, Dr. Tobias Robert, Prof. Dr. J. Hugh Horton and Prof. Dr. Philip G. Jessop

      Article first published online: 3 SEP 2012 | DOI: 10.1002/cssc.201200465

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      The use of inorganic salts to enhance clay settling in aqueous suspensions is a common industrial process. Recycling and/or treatment of this high salinity water after use are necessary environmental and economical practices but are often energetically costly. We propose the use of switchable water, a reversible ionic strength aqueous solvent, as a means to settle clays rapidly with easy recycling of the process water.

    10. Ketonic Decarboxylation Reaction Mechanism: A Combined Experimental and DFT Study (pages 141–151)

      Dr. Angeles Pulido, Borja Oliver-Tomas, Dr. Michael Renz, Dr. Mercedes Boronat and Prof. Avelino Corma

      Article first published online: 30 NOV 2012 | DOI: 10.1002/cssc.201200419

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      This way or that? Monoclinic zirconia has great potential as a catalyst for ketonic decarboxylation of carboxylic acids (see picture). A combined experimental and DFT study shows a route involving a β-keto acid intermediate as the kinetically preferred reaction pathway.

    11. Plasma Synthesis of Polymer-Capped Dye-Sensitised Anatase Nanopowders for Visible-Light-Driven Hydrogen Evolution (pages 152–159)

      Dr. Angela Kruth, Sven Hansen, Dr. Torsten Beweries, Dr. Volker Brüser and Prof. Dr. Klaus-Dieter Weltmann

      Article first published online: 26 NOV 2012 | DOI: 10.1002/cssc.201200408

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      To sensitise and encapsulate: Ru dye-sensitised TiO2 is encapsulated with plasma-polymerised polyallylamine to improve long-term stability under ambient conditions for photocatalytic water splitting. Using a Pd dichloro complex as the reduction catalyst and triethylamine as the electron source, a highly stable long-term performance as well as a small improvement in catalytic activity is achieved. The nanostructure is characterised by TEM as well as UV/Vis and ATR-FTIR spectroscopy.

    12. Characterization of Bio-oil from Hydrothermal Liquefaction of Organic Waste by NMR Spectroscopy and FTICR Mass Spectrometry (pages 160–167)

      Dr. Irene Leonardis, Dr. Stefano Chiaberge, Tiziana Fiorani, Dr. Silvia Spera, Dr. Ezio Battistel, Dr. Aldo Bosetti, Dr. Pietro Cesti, Dr. Samantha Reale and Prof. Francesco De Angelis

      Article first published online: 8 NOV 2012 | DOI: 10.1002/cssc.201200314

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      From waste to fuel: Liquefaction bio-oils can be used as fuel in engines to produce heat and electricity or be upgraded as replacements for diesel and gasoline fuels. An integrated approach based on NMR spectroscopy and MS data is used to characterize a bio-oil obtained from the hydrothermal liquefaction of municipal organic wastes (see picture).

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      Tungsten Carbide Nanoparticles as Efficient Cocatalysts for Photocatalytic Overall Water Splitting (pages 168–181)

      Angel T. Garcia-Esparza, Dr. Dongkyu Cha, Yiwei Ou, Prof. Jun Kubota, Prof. Kazunari Domen and Prof. Kazuhiro Takanabe

      Article first published online: 17 DEC 2012 | DOI: 10.1002/cssc.201200780

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      Platinum replacement: The phase-controlled synthesis of tungsten carbide nanoparticles from the nanoconfinement of a mesoporous graphite C3N4 (mpg-C3N4) reactive template is shown. The nanomaterials catalyze hydrogen evolution/oxidation reactions, but are inactive in the oxygen reduction reaction. Tungsten carbide is an effective cocatalyst for photocatalytic overall water splitting (see picture).

    14. Batchwise and Continuous Nanofiltration of POSS-Tagged Grubbs–Hoveyda-Type Olefin Metathesis Catalysts (pages 182–192)

      Dr. Anna Kajetanowicz, Justyna Czaban, Dr. G. Rajesh Krishnan, Maura Malińska, Prof. Krzysztof Woźniak, Humera Siddique, Dr. Ludmila G. Peeva, Prof. Andrew G. Livingston and Prof. Karol Grela

      Article first published online: 19 OCT 2012 | DOI: 10.1002/cssc.201200466

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      Making metathesis plus nanofiltration POSS-ible: New molecular-weight-enlarged metathesis catalysts, which bear polyhedral oligomeric silsesquioxane (POSS) tags, have been synthesized and characterized. The catalysts can be recovered from the reaction mixture by using nanofiltration techniques and can be reused. The membranes Starmem 228 and PuraMem 280 can be used to successfully separate the catalyst from the post-reaction mixtures.

    15. Mechanical Activation of CaO-Based Adsorbents for CO2 Capture (pages 193–198)

      Maryam Sayyah, Dr. Yongqi Lu, Dr. Richard I. Masel and Prof. Kenneth S. Suslick

      Article first published online: 6 NOV 2012 | DOI: 10.1002/cssc.201200454

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      Having a ball with milling: The reversible cycling of CaO adsorbents to CaCO3 for high-temperature CO2 capture is substantially improved by a mechanochemical approach. MgO has been used as an inert binder to help mitigate CaCO3 sintering. Wet planetary milling of MgO into CaCO3 allows for efficient particle size reduction and effective dispersion of MgO throughout the particles, yielding the most stable sorbents during several cycles of carbonation–calcination.

    16. Conversion of (Ligno)Cellulose Feeds to Isosorbide with Heteropoly Acids and Ru on Carbon (pages 199–208)

      Beau Op de Beeck, Dr. Jan Geboers, Dr. Stijn Van de Vyver, Jonas Van Lishout, Jeroen Snelders, Dr. Wouter J. J. Huijgen, Prof. Dr. Christophe M. Courtin, Prof. Dr. Pierre A. Jacobs and Prof. Dr. Bert F. Sels

      Article first published online: 11 JAN 2013 | DOI: 10.1002/cssc.201200610

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      Biomass to isosorbide: A promising direct route from cellulose to isosorbide is investigated, relying on a joined action of heteropoly acids and Ru on carbon. This strategy enables fast conversions of pure microcrystalline cellulose and impure cellulose pulps into over 50 % and 60 % isosorbide, respectively.

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