ChemSusChem

Cover image for Vol. 6 Issue 6

June 2013

Volume 6, Issue 6

Pages 929–1100

  1. Cover Picture

    1. Top of page
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    3. Cover Profile
    4. Graphical Abstract
    5. Masthead
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    7. Review
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      Cover Picture: Atomic Layer Deposition of High Performance Ultrathin TiO2 Blocking Layers for Dye-Sensitized Solar Cells (ChemSusChem 6/2013) (page 929)

      Do Han Kim, Mariah Woodroof, Kyoungmi Lee and Prof. Gregory N. Parsons

      Version of Record online: 3 JUN 2013 | DOI: 10.1002/cssc.201390023

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      The Cover Image shows the sequential dosing and purging of TiCl4 and H2O in atomic layer deposition (ALD) through step-like pressure changes in an effort to saturate the surface of fluorine doped tin oxide (FTO) glass with each reactant. These ultra-thin and uniform ALD TiO2 films with thicknesses of only 5 nm form a blocking layer on the rough FTO surface to be used in dye-sensitized solar cells (see the report by Kim et al. on page 1014) as the yallow photogenerated electrons to move to the FTO side effectively, thus inhibiting the recombination with holes at the FTO/electrolyte interface.

  2. Cover Profile

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      Atomic Layer Deposition of High Performance Ultrathin TiO2 Blocking Layers for Dye-Sensitized Solar Cells (page 930)

      Do Han Kim, Mariah Woodroof, Kyoungmi Lee and Prof. Gregory N. Parsons

      Version of Record online: 3 JUN 2013 | DOI: 10.1002/cssc.201300468

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      “It was difficult to obtain reliable and consistent results in each thickness.” This and more about the story behind the front cover research can be found on p. 930.

  3. Graphical Abstract

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  4. Masthead

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    1. Masthead: ChemSusChem 6/2013 (page 939)

      Version of Record online: 3 JUN 2013 | DOI: 10.1002/cssc.201390025

  5. News

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  6. Review

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    1. Computational Approaches to the Chemical Conversion of Carbon Dioxide (pages 944–965)

      Prof. Dr. Daojian Cheng, Dr. Fabio R. Negreiros, Dr. Edoardo Aprà and Dr. Alessandro Fortunelli

      Version of Record online: 28 MAY 2013 | DOI: 10.1002/cssc.201200872

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      Calculating transformations: A comprehensive and critical review of the status of research in the field of the chemical conversion of CO2 into carbon forms in a lower oxidation state is presented. Particular attention is devoted to the description of reaction mechanism of CO2 transformation catalyzed by various types of systems (heterogeneous, homogeneous, and electro- and photocatalysts) and to the possible essential role that theoretical and computational approaches can play in this field.

  7. Minireview

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    1. Effect of the Structural Characteristics of Binary Pt–Ru and Ternary Pt–Ru–M Fuel Cell Catalysts on the Activity of Ethanol Electrooxidation in Acid Medium (pages 966–973)

      Prof. Ermete Antolini

      Version of Record online: 6 MAY 2013 | DOI: 10.1002/cssc.201300138

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      Packing a punch: The effect of structural parameters on the ethanol oxidation reaction (EOR) activity of Pt–Ru catalysts is discussed. The EOR activity versus Ru content plots of Pt–Ru catalysts prepared by using different methods go through a maximum, depending on the synthesis method (see image). Alloyed Ru supports ethanol dehydrogenation. Non-alloyed Ru, in the RuOxHy form, supports the oxidation of intermediates species in ethanol oxidation.

  8. Communications

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    1. Dehydrogenation of Dodecahydro-N-ethylcarbazole on Pt(111) (pages 974–977)

      Christoph Gleichweit, Max Amende, Stefan Schernich, Wei Zhao, Michael P. A. Lorenz, Oliver Höfert, Nicole Brückner, Prof. Peter Wasserscheid, Prof. Jörg Libuda, Prof. Hans-Peter Steinrück and Dr. Christian Papp

      Version of Record online: 14 MAY 2013 | DOI: 10.1002/cssc.201300263

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      Sloshing hydrogen: Liquid organic hydrogen carriers are high-boiling organic molecules, which can be reversibly hydrogenated and dehydrogenated in catalytic processes and are, therefore, a promising chemical hydrogen storage material. One of the promising candidates is the pair N-ethylcarbazole/perhydro-N-ethylcarbazole (NEC/H12-NEC). The dehydrogenation and possible side reactions on a Pt(111) surface are evaluated in unprecedented detail.

    2. Continuous-Flow Synthesis of Adipic Acid from Cyclohexene Using Hydrogen Peroxide in High-Temperature Explosive Regimes (pages 978–982)

      Dr. Markus Damm, Bernhard Gutmann and Prof. Dr. C. Oliver Kappe

      Version of Record online: 16 APR 2013 | DOI: 10.1002/cssc.201300197

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      Safe only in a microreactor! The synthesis of adipic acid from cyclohexene by tungstic acid-catalyzed oxidation using hydrogen peroxide following the classical Noyori protocol can be accomplished in good yields with residence times as short as 20 min at 140 °C using a safe and scalable microreactor environment. Under these intensified conditions the use of a phase-transfer catalyst is not required.

    3. Hollow TiO2 Porous Nanosheets: Transformation from ZnO Porous Nanosheets and Application in Photoelectrochemical Cells (pages 983–988)

      Haining Chen, Prof. Liqun Zhu, Qin Hou, Dr. Huicong Liu and Dr. Weiping Li

      Version of Record online: 15 APR 2013 | DOI: 10.1002/cssc.201300099

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      Changing the sheets: Hollow TiO2 porous nanosheets (HTPNs) are prepared on ITO glass through an improved TiO2 polycrystalline shell-assisted cation exchange by using ZnO porous nanosheets (grown by using indirect electrodeposition) as a template. Quantum dot-sensitized solar cells based on HTPNs exhibit a high performance, and other photoelectrochemical devices are expected to be prepared based on HTPNs.

    4. Chemical Conversion of Sugars to Lactic Acid by Alkaline Hydrothermal Processes (pages 989–992)

      Dr. Davide Esposito and Prof. Dr. Markus Antonietti

      Version of Record online: 16 APR 2013 | DOI: 10.1002/cssc.201300092

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      Some like it hot: Lactic acid is an important commodity chemical that is mainly used in the food industry or for the manufacture of biodegradable plastics. A highly efficient strategy for the conversion of carbohydrates from biomass to lactic acid through alkaline hydrolysis in superheated water is presented.

    5. Oligocarbazole-Based Chromophores for Efficient Thin-Film Dye-Sensitized Solar Cells (pages 993–996)

      Samuel De Sousa, Dr. Céline Olivier, Dr. Laurent Ducasse, Dr. Gwenaëlle Le Bourdon, Dr. Lionel Hirsch and Prof. Thierry Toupance

      Version of Record online: 14 MAY 2013 | DOI: 10.1002/cssc.201200975

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      Carb your enthousiasm: Carbazole-based sensitizers with high extinction coefficients are synthesized for application in dye-sensitized solar cells (DSCs). The dyes perform efficiently with both iodine and cobalt electrolytes, showing power conversion efficiencies of up to 5.8 % on TiO2 films of 15 μm thickness, and retaining 90 % of their efficiency in devices with thinner films.

    6. Integrated Chemo-Enzymatic Production of 5-Hydroxymethylfurfural from Glucose (pages 997–1000)

      Svilen P. Simeonov, Jaime A. S. Coelho and Prof. Carlos A. M. Afonso

      Version of Record online: 18 APR 2013 | DOI: 10.1002/cssc.201300176

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      Sweets for my sweet: The production and isolation of 5-hydroxymethylfurfural (HMF) in high yield and purity is demonstrated by using a combination of glucose–fructose isomerization with sweetzyme in wet tetraethylammonium bromide (TEAB) and clean fructose dehydration to HMF catalyzed by using HNO3 under moderate conditions, which allow the reuse of any unreacted glucose and TEAB.

    7. Ruthenium Catalysts for Hydrogenation of Aromatic and Aliphatic Esters: Make Use of Bidentate Carbene Ligands (pages 1001–1005)

      Felix A. Westerhaus, Bianca Wendt, Andreas Dumrath, Gerrit Wienhöfer, Dr. Kathrin Junge and Prof. Matthias Beller

      Version of Record online: 2 MAY 2013 | DOI: 10.1002/cssc.201200825

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      Committed carbenes: The convenient application of bidentate carbene ligands is described for the hydrogenation of carboxylic acid esters. The ligand precursors are easily synthesized through the dimerization of N-substituted imidazoles with diiodomethane. The catalyst is generated in situ and exhibits good activity and functional group tolerance for the hydrogenation of aromatic and aliphatic carboxylic acid esters.

  9. Full Papers

    1. Top of page
    2. Cover Picture
    3. Cover Profile
    4. Graphical Abstract
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    1. Effect of CeO2 Addition to Al2O3 Supports for Pt Catalysts on the Aqueous-Phase Reforming of Glycerol (pages 1006–1013)

      M. M. Rahman, Dr. Tamara L. Church, Prof. Andrew I. Minett and Prof. Andrew T. Harris

      Version of Record online: 24 APR 2013 | DOI: 10.1002/cssc.201200797

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      Pt darn good: Pt catalysts supported on CeO2-doped Al2O3 exhibit higher activity and selectivity towards H2 production in the aqueous-phase reforming of glycerol. Optimization of the CeO2/Al2O3 ratio, higher metal dispersion, and increased active surface area are primarily responsible for the higher glycerol conversion rate and H2 yield.

    2. Atomic Layer Deposition of High Performance Ultrathin TiO2 Blocking Layers for Dye-Sensitized Solar Cells (pages 1014–1020)

      Do Han Kim, Mariah Woodroof, Kyoungmi Lee and Prof. Gregory N. Parsons

      Version of Record online: 29 MAY 2013 | DOI: 10.1002/cssc.201300067

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      Plugging the hole: Atomic layer deposition (ALD) produces ultrathin (<10 nm) blocking layers (BLs) that significantly impede charge recombination in functional dye-sensitized solar cells (DSSCs). This leads to improved photocurrents, open-circuit photovoltages, and fill factors, which increase the overall efficiency from ≈7 % to ≈8.4 % under AM 1.5 G illumination. The 5–10 nm ALD BLs are the thinnest optimized DSSC BLs reported to date.

    3. Intramolecular Hydroalkoxylation of Non-Activated C[DOUBLE BOND]C Bonds Catalysed by Zeolites: An Experimental and Theoretical Study (pages 1021–1030)

      Prof. Elena Pérez-Mayoral, Dr. Ines Matos, Prof. Petr Nachtigall, Miroslav Položij, Prof. Isabel Fonseca, Dr. Dana Vitvarová-Procházková and Prof. Jiří Čejka

      Version of Record online: 23 MAY 2013 | DOI: 10.1002/cssc.201300173

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      The zeolite fantastic: The high efficiency of zeolites MFI, BEA and FAU in the cyclisation of unsaturated alcohols to afford oxygen-containing heterocyclic rings is demonstrated. It is proposed that the efficiency of the catalysts depends on the existence of the so-called dual site, at which a molecule of an unsaturated alcohol can simultaneously interact with two acid sites.

    4. Functionalization of SnO2 Crystals with a Covalently-Assembled Porphyrin Monolayer (pages 1031–1036)

      Dr. Domenico A. Cristaldi and Prof. Antonino Gulino

      Version of Record online: 22 APR 2013 | DOI: 10.1002/cssc.201300149

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      All wrapped up: SnO2 crystals are functionalized with a porphyrin monolayer and the resulting functionalized material is fully characterized. The obtained system shows luminescent properties and has the potential to find application in optical and electronic devices. The two-step procedure for the functionalization of metal-oxide crystals with dye-sensitizers could be applied to a range of metal-oxide semiconductors.

    5. Composite Poly(ethylene oxide) Electrolytes Plasticized by N-Alkyl-N-butylpyrrolidinium Bis(trifluoromethanesulfonyl)imide for Lithium Batteries (pages 1037–1043)

      Morten Wetjen, Dr. Maria Assunta Navarra, Prof. Stefania Panero, Prof. Stefano Passerini, Prof. Bruno Scrosati and Dr. Jusef Hassoun

      Version of Record online: 13 MAY 2013 | DOI: 10.1002/cssc.201300105

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      Electrolyte right! A new and attractive electrolyte based on polyethylene oxide and N-butyl-N-ethyl-pyrrolidinium bis(trifluoromethanesulfonyl)imide ionic liquid as plasticizer shows high conductivity at medium to low temperatures. This allows its employment in a solid polymer lithium battery using LiFePO4 as the cathode and its efficient operation at temperatures of about 50 °C.

    6. Catalytic Characteristics of AgCu Bimetallic Nanoparticles in the Oxygen Reduction Reaction (pages 1044–1049)

      Kihyun Shin, Dr. Da Hye Kim and Prof. Hyuck Mo Lee

      Version of Record online: 3 MAY 2013 | DOI: 10.1002/cssc.201201001

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      AgCu (alloy) nanoparticle: The adsorption energy of oxygen and the activation energy of oxygen dissociation are important factors that determine the performance of oxygen reduction reaction catalysts. We propose the utilization of a AgCu-alloy nanoparticle system as a potential highly efficient catalyst in this setting because it possesses good catalytic properties and prevents Cu oxidation.

    7. Reactivity of Azole Anions with CO2 from the DFT Perspective (pages 1050–1056)

      Huarong Tang and Dr. Chao Wu

      Version of Record online: 2 MAY 2013 | DOI: 10.1002/cssc.201200986

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      Catch me if you can: Azole anions represent a key component in CO2 absorption materials. A variety of different azole anions have been investigated for their reactivity with CO2 by using DFT calculations and a Langmuir adsorption model. Unlike SO2, multi-site CO2 absorption does not occur for azole anions under normal conditions. This study provides insight into designing azole-based CO2-capture materials.

    8. Superhydrophobic Activated Carbon-Coated Sponges for Separation and Absorption (pages 1057–1062)

      Hanxue Sun, Prof. An Li, Zhaoqi Zhu, Dr. Weidong Liang, Dr. Xinhong Zhao, Prof. Peiqing La and Prof. Weiqiao Deng

      Version of Record online: 3 MAY 2013 | DOI: 10.1002/cssc.201200979

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      Supersponge, save the world! Superhydrophobic activated carbon-coated sponges show good selectivity, recyclability, and absorbencies ranging from 2695 to 8586 wt % for a wide range of organic solvents and oils. These materials may have useful applications especially in the fields of oil-spill cleanup and water treatment.

    9. Nafion-Resin-Modified Mesocellular Silica Foam Catalyst for 5-Hydroxymethylfurfural Production from D-Fructose (pages 1063–1069)

      Zhen Huang, Wenya Pan, Haibo Zhou, Feng Qin, Prof. Hualong Xu and Prof. Wei Shen

      Version of Record online: 13 MAY 2013 | DOI: 10.1002/cssc.201200967

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      Valuable sugars: Nafion-resin-functionalized mesocellular silica foam (MCF) is a strong solid acid that can be prepared through an impregnation method. By using this method, Nafion is well-dispersed in the ultra-large cells of MCFs. This material can easily be reused and exhibits high efficiency and selectivity for the acid-catalyzed dehydration of D-fructose to 5-hydroxymethylfurfural under mild conditions.

    10. Polymer Bulk Heterojunction Solar Cells with PEDOT:PSS Bilayer Structure as Hole Extraction Layer (pages 1070–1075)

      Wanjung Kim, Namhun Kim, Jung Kyu Kim, Dr. Insun Park, Dr. Yeong Suk Choi, Dr. Dong Hwan Wang, Prof. Heeyeop Chae and Prof. Jong Hyeok Park

      Version of Record online: 9 MAY 2013 | DOI: 10.1002/cssc.201200950

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      Two layers are better than one: The systematic increase in power conversion efficiency of polymer solar cells (PSCs) is demonstrated by considering the charge carrier transfer and electric field strength of a device. The unexpected and greatly enhanced power conversion efficiency of PSCs is reported, which can be accomplished by using a PEDOT:PSS hole extraction bilayer. Two different model systems are studied: P3HT:PC60BM and PCDTBT:PC70BM.

    11. CO2 Sorbents with Scaffold-like Ca[BOND]Al Layered Double Hydroxides as Precursors for CO2 Capture at High Temperatures (pages 1076–1083)

      Dr. Po-Hsueh Chang, Tai-Jung Lee, Dr. Yen-Po Chang and Prof. San-Yuan Chen

      Version of Record online: 3 MAY 2013 | DOI: 10.1002/cssc.201200910

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      Caught in a web: A Ca[BOND]Al layered double hydroxide-based scaffold-like network is synthesized in the presence of hexadecyl trimethyl ammonium bromide (CTAB) by using a sol–gel process with Al(OiP)3 and Ca(NO3)2 as precursors. The calcined Ca[BOND]Al[BOND]NO3 layered double hydroxides display rapid CO2 absorption kinetics in addition to a long-term cyclic operation in a high-temperature environment.

    12. Large-Scale Production of Nanographene Sheets with a Controlled Mesoporous Architecture as High-Performance Electrochemical Electrode Materials (pages 1084–1090)

      Haitao Zhang, Dr. Xiong Zhang, Dr. Xianzhong Sun, Dacheng Zhang, He Lin, Changhui Wang, Hongjin Wang and Prof. Yanwei Ma

      Version of Record online: 3 MAY 2013 | DOI: 10.1002/cssc.201200904

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      Nanographene electrodes are go: The large-scale production of nanographene with a controlled mesoporous architecture is achieved by a new burn–quench method, which involves the ignition of Mg ribbons in CO2 followed by in situ quenching. Nanographene with a mesoporous architecture has a high surface area and high conductivity.

    13. New Insights into the Oxygen Reduction Reaction Mechanism on Pt (111): A Detailed Electrochemical Study (pages 1091–1100)

      Ana M. Gómez-Marín and Prof. Dr. Juan M. Feliu

      Version of Record online: 2 MAY 2013 | DOI: 10.1002/cssc.201200847

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      A radical idea! The oxygen reduction reaction on Pt (111) in the high potential region is not inhibited by the initial oxidized surface states. Instead, the reduction of a soluble intermediate species apparently is the rate determining step.

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