ChemSusChem

Cover image for Vol. 6 Issue 11

November 2013

Volume 6, Issue 11

Pages 2023–2197

  1. Cover Pictures

    1. Top of page
    2. Cover Pictures
    3. Cover Profile
    4. Graphical Abstract
    5. Masthead
    6. News
    7. Highlights
    8. Essay
    9. Communications
    10. Full Papers
    1. You have free access to this content
      Cover Picture: Carbon Nitride for the Selective Oxidation of Aromatic Alcohols in Water under Visible Light (ChemSusChem 11/2013) (page 2023)

      Baihua Long, Prof. Zhengxin Ding and Prof. Xinchen Wang

      Article first published online: 29 OCT 2013 | DOI: 10.1002/cssc.201301097

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      Aldehydes are key intermediates for the industrial synthesis of bulk and fine chemicals. The front cover image of issue 11/2013, by Baihu Long, Zhengxin Ding, and Xincheng Wang at Fuzhou University, illustrates a metal-free carbon nitride photocatalyst that selectively transforms aromatic alcohols into the corresponding aldehydes. The reactions run in water under visible light illumination, in an atmosphere of oxygen. Two distinct characteristics of carbon nitride, namely its unique electronic structure and its very high chemical stability, are essential for enabling a choice from a wide range of chemical protocols to promote photoredox catalysis in water, as exemplified here by cooperative catalysis involving Brønsted acids. These findings have important conceptual and practical implications for other applications in the fine-chemicals industry. More detail is given in Wang et al.′s Communication on page 2074 (DOI: 10.1002/cssc.201300360), while more information about the research group is available in the Cover Profile (DOI: 10.1002/cssc.201301098).

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      Back Cover: Conversion of Cellulose into Isosorbide over Bifunctional Ruthenium Nanoparticles Supported on Niobium Phosphate (ChemSusChem 11/2013) (page 2198)

      Dr. Peng Sun, Xiangdong Long, Hao He, Prof. Dr. Chungu Xia and Prof. Dr. Fuwei Li

      Article first published online: 25 OCT 2013 | DOI: 10.1002/cssc.201301044

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      The back cover image shows the production of isosorbide from the one-pot hydrolytic hydrogenation and dehydration of inedible cellulose. Dr Fuwei Li and co-workers show that isosorbide production can be achieved under hydrothermal conditions over a recyclable ruthenium catalyst supported on mesoporous niobium phosphate without the addition of soluble acids. This efficient and sustainable protocol could close the carbon cycle as a result of plants taking up CO2 generated from the end products. More details can be found in the Full Paper by Sun et. al on page 2190 (DOI: 10.1002/cssc.201300701).

  2. Cover Profile

    1. Top of page
    2. Cover Pictures
    3. Cover Profile
    4. Graphical Abstract
    5. Masthead
    6. News
    7. Highlights
    8. Essay
    9. Communications
    10. Full Papers
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      Carbon Nitride for the Selective Oxidation of Aromatic Alcohols in Water under Visible Light (page 2024)

      Baihua Long, Prof. Zhengxin Ding and Prof. Xinchen Wang

      Article first published online: 8 NOV 2013 | DOI: 10.1002/cssc.201301098

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      “Green chemistry necessitates the development of new synthetic methods, including ones that enable selective transformations to be conducted in a more environmentally benign manner.” This and more about the story behind the research that inspired the cover image at 10.1002/cssc.201301098. View the front cover at 10.1002/cssc.201301097.

  3. Graphical Abstract

    1. Top of page
    2. Cover Pictures
    3. Cover Profile
    4. Graphical Abstract
    5. Masthead
    6. News
    7. Highlights
    8. Essay
    9. Communications
    10. Full Papers
    1. Graphical Abstract: ChemSusChem 11/2013 (pages 2025–2033)

      Article first published online: 8 NOV 2013 | DOI: 10.1002/cssc.201390038

  4. Masthead

    1. Top of page
    2. Cover Pictures
    3. Cover Profile
    4. Graphical Abstract
    5. Masthead
    6. News
    7. Highlights
    8. Essay
    9. Communications
    10. Full Papers
    1. Masthead: ChemSusChem 11/2013 (pages 2034–2035)

      Article first published online: 8 NOV 2013 | DOI: 10.1002/cssc.201390039

  5. News

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

    1. Top of page
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    3. Cover Profile
    4. Graphical Abstract
    5. Masthead
    6. News
    7. Highlights
    8. Essay
    9. Communications
    10. Full Papers
    1. Continuous Mesoporous Titania Nanocrystals: Their Growth in Confined Space and Scope for Application (pages 2039–2041)

      Dr. Saikat Dutta and Prof. Dr. Asim Bhaumik

      Article first published online: 4 SEP 2013 | DOI: 10.1002/cssc.201300423

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      Enjoying the single lifestyle: With an overwhelming efficiency compared to thermally sintered preformed nanocrystals, mesoporous single crystals (MSCs) of TiO2 constitute a new class of semiconductor materials for low-cost solar power, solar fuel, photocatalysis, and energy storage applications. This Highlight explores the benefits of template-directed seed-mediated growth in the confined space of a preseeded mesoporous template, and possible research avenues for further improvements.

    2. Mechanocatalytic Deconstruction of Cellulose: An Emerging Entry into Biorefinery (pages 2042–2044)

      Dr. Qinghua Zhang and Dr. François Jérôme

      Article first published online: 7 OCT 2013 | DOI: 10.1002/cssc.201300765

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      Deconstructing cellulose: This highlight presents an emerging concept dealing with the mechanocatalytic deconstruction of biopolymers including cellulose, lignin, and lignocellulosic biomass. This dry treatment of biomass is expected to open new horizons in the field of biomass processing. In particular, mechanocatalysis is now considered as a promising entry into biorefinery.

  7. Essay

    1. Top of page
    2. Cover Pictures
    3. Cover Profile
    4. Graphical Abstract
    5. Masthead
    6. News
    7. Highlights
    8. Essay
    9. Communications
    10. Full Papers
    1. Scarcity of Rare Earth Elements (pages 2045–2055)

      M. A. de Boer and K. Lammertsma

      Article first published online: 5 SEP 2013 | DOI: 10.1002/cssc.201200794

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      Urban mining of rare earth elements: Rare earth elements (REEs) are important resources for green and high-tech technologies. Export quotas, a price increase by a factor of ten, and geopolitical and sustainability concerns lead to the reopening of mines. The increased demand and decreased export will lead to a misbalance of four REEs (Nd, Tb, Dy, Pr) on the short term; therefore, as no alternatives are available yet, it is necessary to recycle these elements from electronic waste.

  8. Communications

    1. Top of page
    2. Cover Pictures
    3. Cover Profile
    4. Graphical Abstract
    5. Masthead
    6. News
    7. Highlights
    8. Essay
    9. Communications
    10. Full Papers
    1. Infrared Sensitizers in Titania-Based Dye-Sensitized Solar Cells using a Dimethylferrocene Electrolyte (pages 2056–2060)

      Dr. Torben Daeneke, Dr. Katja Gräf, Dr. Scott E. Watkins, Prof. Mukundan Thelakkat and Prof. Udo Bach 

      Article first published online: 5 SEP 2013 | DOI: 10.1002/cssc.201300582

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      Vide infra: Two boron-dipyrromethene (BODIPY)-type infrared sensitizers are investigated for use in titania-based dye-sensitized solar cells (DSCs). The DSCs use a solution of dimethylferrocene (Me2Fc) in nitromethane as electrolyte. The titania conduction band edge is fine-tuned by adding lithium ions from LiTFSI, while the choice of dimethylferrocene as redox shuttle provides the ideal driving force for dye regeneration, allowing the BODIPY-based DSCs to reach unprecedented quantum efficiencies in the near-infrared.

    2. Oxidative Methane Reforming with an Intelligent Catalyst: Sintering-Tolerant Supported Nickel Nanoparticles (pages 2061–2065)

      Jie Deng, Mengdie Cai, Wenjing Sun, Xuemei Liao, Prof. Wei Chu and Prof. Xiu Song Zhao

      Article first published online: 7 OCT 2013 | DOI: 10.1002/cssc.201300452

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      Smart Catalyst: The cyclical diffusion of nanometer-sized nickel clusters into and out of the perovskite structure under elevated temperature and reducing and oxidizing atmosphere could in situ redeliver and redisperse Ni, thereby reinforcing the anti-coking and -sintering of Ni during oxidative reforming of CH4.

    3. On the Brønsted Acid-Catalyzed Homogeneous Hydrolysis of Furans (pages 2066–2068)

      Nima Nikbin, Dr. Stavros Caratzoulas and Prof. Dr. Dionisios G. Vlachos

      Article first published online: 4 SEP 2013 | DOI: 10.1002/cssc.201300432

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      Furan affairs: Electronic structure calculations of the homogeneous Brønsted acid-catalyzed hydrolysis of 2,5-dimethylfuran show that proton transfer to the β-position is rate-limiting and provides support that the hydrolysis follows general acid catalysis. By means of projected Fukui indices, we show this to be the case for unsubstituted, 2-, and 2,5-substituted furans with electron-donating groups.

    4. Dye-Sensitized Solar Cells based on Organic Dual-Channel Anchorable Dyes with Well-Defined Core Bridge Structures (pages 2069–2073)

      Kang Deuk Seo, Ban Seok You, In Taek Choi, Dr. Myung Jong Ju, Mi You, Prof. Dr. Hong Seok Kang and Prof. Dr. Hwan Kyu Kim

      Article first published online: 28 AUG 2013 | DOI: 10.1002/cssc.201300365

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      In stereo, where available: A new approach towards dye-sensitized solar cells is based on dianchoring structural motifs with two donors, two acceptors, and a core bridge donor as a spacer. Their high molar absorption coefficients result in favorable light-harvesting efficiencies for DSSCs based on these dyes. A high conversion efficiency of 4.90 % is achieved when using dye DC4, containing a core bridge carbazole unit, with a multifunctional coadsorbent.

    5. Carbon Nitride for the Selective Oxidation of Aromatic Alcohols in Water under Visible Light (pages 2074–2078)

      Baihua Long, Prof. Zhengxin Ding and Prof. Xinchen Wang

      Article first published online: 26 AUG 2013 | DOI: 10.1002/cssc.201300360

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      The selective oxidation of aromatic alcohols in water is achieved by using a carbon nitride (CN) catalyst, dioxygen, and visible light. The unique electronic structure of CN avoids the direct formation of hydroxyl radicals, which typically cause the total oxidation of organics. The chemical stability of CN allows several chemical protocols for photoredox catalysis in water, as exemplified by cooperative catalysis involving Brønsted acids. This leads to a new, green pathway for diverse organic transformations using sunlight and water.

    6. Stabilizing the Imidazolium Cation in Hydroxide-Exchange Membranes for Fuel Cells (pages 2079–2082)

      Dr. Junhua Wang, Prof. Dr. Shuang Gu, Robert B. Kaspar, Bingzi Zhang and Prof. Dr. Yushan Yan

      Article first published online: 22 AUG 2013 | DOI: 10.1002/cssc.201300285

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      Stable and able: The hydroxide-conducting cationic functional group used in the hydroxide-exchange membranes of fuel cells is key to controlling chemical stability and solubility. A new imidazolium cation, 1,4,5-trimethyl-2-(2,4,6-trimethoxyphenyl)imidazolium, is designed to take advantage of both strong electron-donation properties and steric hindrance. Synergy between these two effects leads to an efficient hydroxide-exchange membrane, with increased alkaline stability and improved OH conductivity.

    7. Simulated Moving Bed Chromatography: Separation and Recovery of Sugars and Ionic Liquid from Biomass Hydrolysates (pages 2083–2089)

      Benjamin R. Caes, Thomas R. Van Oosbree, Fachuang Lu, Prof. John Ralph, Prof. Christos T. Maravelias and Prof. Ronald T. Raines

      Article first published online: 12 AUG 2013 | DOI: 10.1002/cssc.201300267

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      Separation from bed, not board: Simulated moving bed chromatography, a continuous separation method, enables the nearly quantitative recovery of sugar products and ionic liquid solvent from chemical hydrolysates of biomass. The ensuing sugars support microbial growth, and the residual lignin from the process is intact.

    8. Direct Synthesis of Sorbitol and Glycerol from Cellulose over Ionic Ru/Magnetite Nanoparticles in the Absence of External Hydrogen (pages 2090–2094)

      Alina Negoi, Ioan Teodor Trotus, Prof. Olimpia Mamula Steiner, Dr. Madalina Tudorache, Dr. Victor Kuncser, Dr. Dan Macovei, Prof. Vasile I. Parvulescu and Prof. Simona M. Coman

      Article first published online: 23 SEP 2013 | DOI: 10.1002/cssc.201300554

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      A sweet catalyst: A catalyst formed of Ru/functionalized silica-coated magnetite nanoparticles is highly efficient in the one-pot production of sorbitol and glycerol, starting from cellulose and in the absence of an external hydrogen source. The ease of recoverability of the catalyst from the solid residues, and its reuse without loss of activity or selectivity for several runs, is an important green element of the process.

  9. Full Papers

    1. Top of page
    2. Cover Pictures
    3. Cover Profile
    4. Graphical Abstract
    5. Masthead
    6. News
    7. Highlights
    8. Essay
    9. Communications
    10. Full Papers
    1. Origin of Photocatalytic Activity in Continuous Gas Phase CO2 Reduction over Pt/TiO2 (pages 2095–2102)

      Antonio Bazzo and Dr. Atsushi Urakawa

      Article first published online: 26 AUG 2013 | DOI: 10.1002/cssc.201300307

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      Always look on the dark side of life! Two distinct activities, steady-state and transient, in the continuous photocatalytic reduction of humidified gaseous CO2 to CH4 and H2 over Pt/TiO2 under UV irradiation are identified, by monitoring the product concentrations with the time-resolution of seconds by means of mass spectrometry. Reactivation of the transient activity occurs under dark conditions. The reactivation mechanism is explained by performing an in situ diffuse reflectance infrared Fourier transform spectroscopy study.

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      Cu/MgAl2O4 as Bifunctional Catalyst for Aldol Condensation of 5-Hydroxymethylfurfural and Selective Transfer Hydrogenation (pages 2103–2110)

      Kristina Pupovac and Prof. Dr. Regina Palkovits

      Article first published online: 12 SEP 2013 | DOI: 10.1002/cssc.201300414

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      Set your catalyst noble-metal free! Copper supported on mesoporous magnesium aluminate allows an efficient aldol condensation of 5-hydroxymethylfurfural with acetone, followed by selective hydrogenation to 3-hydroxybutyl-5-methylfuran. This noble-metal-free catalyst is active under hydrogen pressure and in transfer hydrogenation utilizing 2-propanol as a solvent.

    3. Yolk–Shell, Hollow, and Single-Crystalline ZnCo2O4 Powders: Preparation Using a Simple One-Pot Process and Application in Lithium-Ion Batteries (pages 2111–2116)

      Seung Ho Choi and Prof. Yun Chan Kang

      Article first published online: 31 JUL 2013 | DOI: 10.1002/cssc.201300300

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      Heroes in a double shell: Double-shelled ZnCo2O4 yolk–shell powder with a complex composition is prepared directly from the sucrose-containing spray solution by using spray pyrolysis within a short residence time. The yolk–shell ZnCo2O4 powder displayed better cycling and rate performances than those of the hollow and single-crystalline powders, and have good electrochemical properties even at high current densities.

    4. Efficiency Enhancement of Dye-Sensitized Solar Cells by the Addition of an Oxidizing Agent to the TiO2 Paste (pages 2117–2123)

      Kwan-Woo Ko, Minoh Lee, Prof. S. S. Sekhon, Suresh Kannan Balasingam, Dr. Chi-Hwan Han and Prof. Yongseok Jun

      Article first published online: 17 SEP 2013 | DOI: 10.1002/cssc.201300280

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      Cut and paste Addition of a strong oxidizing agent (3,5-dinitrosalicylic acid) to the TiO2 paste facilitates the exothermic burning of organic binders during the high temperature calcination process, resulting in smaller amounts of residual carbon. This reduced carbon content facilitates the adsorption of more dye molecules on the TiO2 surface and results in a higher efficiency of the cell.

    5. Efficient Dye-Sensitized Solar Cells Using a Tetramethylthiourea Redox Mediator (pages 2124–2131)

      Yeru Liu, Dr. James R. Jennings and Prof. Qing Wang

      Article first published online: 8 AUG 2013 | DOI: 10.1002/cssc.201300238

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      Mediator to dye for! A tetramethylthiourea redox mediator in conjunction with an indoline dye (D205) yields power conversion efficiencies of up to 7.6 % under AM 1.5G 1 sun illumination when used in dye-sensitized solar cells. This success is attributed to the superior light harvesting, efficient sensitizer regeneration, and fast charge-transfer kinetics at the counter electrode.

    6. Furfural Production by ‘Acidic Steam Stripping’ of Lignocellulose (pages 2132–2136)

      Dr. Jeroen van Buijtenen, Prof. Jean-Paul Lange, Dr. Leticia Espinosa Alonso, Wouter Spiering, Rob F. Polmans and Rene J. Haan

      Article first published online: 31 JUL 2013 | DOI: 10.1002/cssc.201300234

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      Stripping away the inessential: Furfural is produced with approximately 60 mol % yield upon stripping bagasse with a gaseous stream of HCl/steam. Critical process aspects such as effluent recycling, metallurgy and product recovery are discussed.

    7. Drinking Water Purification by Electrosynthesis of Hydrogen Peroxide in a Power-Producing PEM Fuel Cell (pages 2137–2143)

      Winton Li, Dr. Arman Bonakdarpour, Prof. Dr. Előd Gyenge and Prof. Dr. David P. Wilkinson

      Article first published online: 12 SEP 2013 | DOI: 10.1002/cssc.201300225

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      What a treat! The electroreduction of oxygen to H2O2 at the cathode of a proton exchange membrane (PEM) fuel cell could be a solution for purifying drinking water on small scales. A fuel cell reactor is operated with a continuous flow of carrier water through the cathode to remove the product H2O2. The impact of the cobalt–carbon composite cathode catalyst loading, Teflon content in the cathode gas diffusion layer, and cathode carrier water flowrate on the production of H2O2 are examined.

    8. Polymer-free Vertical Transfer of Silicon Nanowires and their Application to Energy Storage (pages 2144–2148)

      Dr. Han-Jung Kim, Dr. Jihye Lee, Sang Eon Lee, Wanjung Kim, Hwan Jin Kim, Dr. Dae-Geun Choi and Prof. Jong Hyeok Park

      Article first published online: 12 SEP 2013 | DOI: 10.1002/cssc.201300202

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      Standing up: A fabrication method for silicon nanowire (SiNW) assemblies for lithium-ion-battery (LIB) electrodes that require no additional support or conductive materials such as polymeric binder or carbon black is reported. When evaluated as an LIB anode without using conventional polymeric binder and a conducting additive, the transferred vertically aligned SiNWs showed a high specific capacity and excellent rate performance.

    9. Synthesis of 9-Oxononanoic Acid, a Precursor for Biopolymers (pages 2149–2156)

      Konrad B. Otte, Marko Kirtz, Dr. Bettina M. Nestl and Prof. Dr. Bernhard Hauer

      Article first published online: 9 AUG 2013 | DOI: 10.1002/cssc.201300183

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      Access to biopolymers: Starting from linoleic acid, a multi-enzymatic one-pot process is successfully applied to produce 9-oxononanoic acid in high yield. The enzymatic cascade reaction consists of a lipoxygenase, which introduces a hydroperoxy group into the polyunsaturated fatty acids, and a hydroperoxide lyase, which performs the cleavage reaction on the nascent hydroperoxy moiety.

    10. Molecular Relaxations in Magnesium Polymer Electrolytes via GHz Broadband Electrical Spectroscopy (pages 2157–2160)

      Dr. Michele Piccolo, Dr. Guinevere A. Giffin, Dr. Keti Vezzù, Dr. Federico Bertasi, Prof. Piergiorgio Alotto, Prof. Massimo Guarnieri and Prof. Vito Di Noto

      Article first published online: 18 SEP 2013 | DOI: 10.1002/cssc.201300145

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      Setting in motion: An electrolyte that can transfer magnesium ions efficiently is presented. This electrolyte is based on polyethylene glycol 400 and a polymeric form of the δ-MgCl2 magnesium salt. GHz broadband electrical spectroscopy (G-BES) is used to investigate the molecular relaxations and the interactions occurring within the system. The information obtained by G-BES is used in the study of the conduction mechanism.

    11. Predicting Cellulose Solvating Capabilities of Acid–Base Conjugate Ionic Liquids (pages 2161–2169)

      Arno Parviainen, Dr. Alistair W. T. King, Dr. Ilpo Mutikainen, Dr. Michael Hummel, Christoph Selg, Lauri K. J. Hauru, Prof. Dr. Herbert Sixta and Prof. Dr. Ilkka Kilpeläinen

      Article first published online: 18 SEP 2013 | DOI: 10.1002/cssc.201300143

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      Distillation and solubility: Rational design of protic ionic liquids that are both distillable (as a means of recycling) and are excellent solvents for cellulose has been achieved. Ab initio and experimental studies highlight the role of a protic cation in the thermodynamics of cellulose dissolution. Structures described herein are comparable with commercial materials.

    12. A Simple Synthetic Route to Obtain Pure Trans-Ruthenium(II) Complexes for Dye-Sensitized Solar Cell Applications (pages 2170–2180)

      Dr. Claudia Barolo, Dr. Jun-Ho Yum, Dr. Emma Artuso, Dr. Nadia Barbero, Dr. Davide Di Censo, Dr. Maria Grazia Lobello, Dr. Simona Fantacci, Dr. Filippo De Angelis, Prof. Michael Grätzel, Prof. Mohammed Khaja Nazeeruddin and Prof. Guido Viscardi

      Article first published online: 7 AUG 2013 | DOI: 10.1002/cssc.201200973

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      Pure­ trans-Ru complexes for DSSCs: A facile synthetic route to obtain functionalized quaterpyridine ligand and its trans-dithiocyanato Ru complex, based on a microwave-assisted procedure, is presented. The highly pure complex exhibits panchromatic response throughout the visible region and shows a high overall photovoltaic conversion efficiency at standard AM 1.5 sunlight, the best efficiency reported up to now for tetradentate ligand-based RuII dyes.

    13. Solid–Solid Heterogeneous Catalysis: The Role of Potassium in Promoting the Dehydrogenation of the Mg(NH2)2/2 LiH Composite (pages 2181–2189)

      Dr. Jianhui Wang, Prof. Ping Chen, Prof. Hongge Pan, Prof. Zhitao Xiong, Dr. Mingxia Gao, Dr. Guotao Wu, Dr. Chu Liang, Cao Li, Bo Li and Jieru Wang

      Article first published online: 31 JUL 2013 | DOI: 10.1002/cssc.201200885

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      Potassium is in the loop: The introduction of potassium to the Mg(NH2)2/2 LiH composite evolves intermediates of K2Mg(NH2)4, Li3K(NH2)4, and KH, which circularly transform between each other to create a more energy-favorable pathway for dehydrogenation, and thus contributes to the overall kinetic enhancement.

    14. Conversion of Cellulose into Isosorbide over Bifunctional Ruthenium Nanoparticles Supported on Niobium Phosphate (pages 2190–2197)

      Dr. Peng Sun, Xiangdong Long, Hao He, Prof. Dr. Chungu Xia and Prof. Dr. Fuwei Li

      Article first published online: 20 SEP 2013 | DOI: 10.1002/cssc.201300701

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      Reap what ye isosorbide: A high yield of isosorbide from the one-pot hydrolytic hydrogenation and dehydration of inedible cellulose is achieved under hydrothermal conditions over a recyclable ruthenium catalyst supported on mesoporous niobium phosphate without the addition of soluble acids. This efficient and sustainable protocol could close the carbon cycle as a result of plants taking up CO2 generated from the end products.

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