ChemSusChem

Cover image for Vol. 5 Issue 10

October 2012

Volume 5, Issue 10

Pages 1849–2087

  1. Cover Pictures

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    1. Cover Picture: Role of Water in the Chlorine Evolution Reaction at RuO2-Based Electrodes—Understanding Electrocatalysis as a Resonance Phenomenon (ChemSusChem 10/2012) (page 1849)

      Aleksandar R. Zeradjanin, Nadine Menzel, Prof. Dr. Peter Strasser and Prof. Dr. Wolfgang Schuhmann

      Article first published online: 15 OCT 2012 | DOI: 10.1002/cssc.201290041

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      The cover image shows how the reaction path of the Cl2 evolution reaction (CER) is investigated by combining electrochemical and spectroscopic methods, as reported by Schuhmann et al. on page 1897. Oxidation and reconstruction of the catalyst surface during CER is a consequence of the interaction between RuO2 and water. The solvent is crucial in the formation of an oxygen-containing hydrophilic layer, which is a key prerequisite for electrocatalytic Cl2 formation. New insights in the general understanding of electrocatalysis are obtained utilizing the vibration frequencies of the crystal lattice as a dynamic catalytic descriptor, instead of thermodynamic descriptors such as the adsorption energy of intermediates. Interpretation of the derived “volcano”-curve suggests that electrocatalysis is governed by a resonance phenomenon.

    2. Inside Cover: (ChemSusChem 10/2012) (page 1850)

      Article first published online: 15 OCT 2012 | DOI: 10.1002/cssc.201290042

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      The inside cover picture shows a promising candidate for efficient CO2 capture demonstrated by Dai et al. Porous, nitrogen-doped carbons can be facilely synthesized from task-specific ionic liquids (TSILs) via high-yield carbonization reactions. These nitrogen-doped carbonaceous materials exhibit an exceptional CO2 absorption capacity because of the strong interaction between CO2 and the nitrogen-containing basic sites within the carbon frameworks.

  2. Graphical Abstract

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    1. Graphical Abstract: ChemSusChem 10/2012 (pages 1851–1859)

      Article first published online: 15 OCT 2012 | DOI: 10.1002/cssc.201290043

  3. News

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  4. Review

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    1. Synthesis and Applications of Graphene-Based TiO2 Photocatalysts (pages 1868–1882)

      Lling-Lling Tan, Dr. Siang-Piao Chai and Prof. Abdul Rahman Mohamed

      Article first published online: 14 SEP 2012 | DOI: 10.1002/cssc.201200480

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      Power in the mix: The incorporation of TiO2 onto graphene is gaining tremendous research interest as it presents the opportunity to simultaneously cover all mechanisms of photocatalytic enhancement. Herein, the theoretical framework, synthetic strategies for the preparation and modification, and applications of these photocatalysts are reviewed, with particular attention on the photodegradation of pollutants and photocatalytic water splitting for hydrogen generation.

  5. Communications

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    1. Oxidative Pyrolysis of Polystyrene into Styrene Monomers in an Autothermal Fixed-Bed Catalytic Reactor (pages 1883–1887)

      Hui Sun, Corey Rosenthal and Prof. Lanny D. Schmidt

      Article first published online: 14 SEP 2012 | DOI: 10.1002/cssc.201200412

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      Styrene monomer recovery: A selective stream of styrene from fast pyrolysis of polystyrene is obtained with an autothermal fixed-bed reactor containing noble-metal (Rh, Pt) catalysts. Autothermal fast pyrolysis of polystyrene is an efficient means of recovering monomers from waste polystyrene in a continuous, high-throughput process without external heating.

    2. Practical and Efficient Iridium Catalysis for Benzannulation: An Entry To Isoindolines (pages 1888–1891)

      Dr. Anne-Laure Auvinet, Dr. Mehdi Ez-Zoubir, Dr. Maxime R. Vitale, Dr. Jack A. Brown, Dr. Véronique Michelet and Dr. Virginie Ratovelomanana-Vidal

      Article first published online: 23 SEP 2012 | DOI: 10.1002/cssc.201200443

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      Iridium(III) catalysis provides a convenient and general method for the synthesis of isoindolines via [2+2+2] cycloaddition reactions of diynes and alkynes. The reaction proceeds smoothly in environmentally benign and non-distilled isopropyl alcohol, providing highly functionalized aromatic compounds in moderate to excellent yields.

    3. From Alkyl Aromatics to Aromatic Esters: Efficient and Selective C[BOND]H Activation Promoted by a Bimetallic Heterogeneous Catalyst (pages 1892–1896)

      Hongli Liu, Gongzhou Chen, Prof. Huanfeng Jiang, Prof. Yingwei Li and Prof. Rafael Luque

      Article first published online: 23 SEP 2012 | DOI: 10.1002/cssc.201200611

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      Oxidizing aromatics: We report an operationally simple and green catalytic oxidative esterification approach that selectively converts methyl aromatics to aromatic carboxylates utilizing a highly stable, active, and reusable heterogeneous bimetallic Au–Pd catalyst and molecular oxygen as benign oxidant without requiring any additives.

  6. Full Papers

    1. Top of page
    2. Cover Pictures
    3. Graphical Abstract
    4. News
    5. Review
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    1. Role of Water in the Chlorine Evolution Reaction at RuO2-Based Electrodes—Understanding Electrocatalysis as a Resonance Phenomenon (pages 1897–1904)

      Aleksandar R. Zeradjanin, Nadine Menzel, Prof. Dr. Peter Strasser and Prof. Dr. Wolfgang Schuhmann

      Article first published online: 14 AUG 2012 | DOI: 10.1002/cssc.201200193

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      Water powered! The reaction path of the Cl2 evolution reaction (CER) is investigated by combining electrochemical and spectroscopic methods. Oxidation and reconstruction of the catalyst surface during CER is a consequence of the interaction between RuO2 and water. Interpretation of the derived volcano curve suggests that electrocatalysis is governed by a resonance phenomenon (see picture).

    2. Evaluation of the Catalytic Performance of Gas-Evolving Electrodes using Local Electrochemical Noise Measurements (pages 1905–1911)

      Aleksandar R. Zeradjanin, Dr. Edgar Ventosa, Dr. Alexander S. Bondarenko and Prof. Dr. Wolfgang Schuhmann

      Article first published online: 23 SEP 2012 | DOI: 10.1002/cssc.201200262

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      Tip of the iceberg: Positioned scanning electrochemical microscopy tips are used to determine the characteristic frequency of gas-bubble detachment from ruthenium-based dimensionally stable anodes at different applied potentials (see picture). Geometrical factors and optimized microstructures of the electrode surface are essential for improving the overall catalytic activity for industrial applications.

    3. Efficient CO2 Capture by Porous, Nitrogen-Doped Carbonaceous Adsorbents Derived from Task-Specific Ionic Liquids (pages 1912–1917)

      Xiang Zhu, Dr. Patrick C. Hillesheim, Shannon M. Mahurin, Prof. Congmin Wang, Chengcheng Tian, Suree Brown, Dr. Huimin Luo, Dr. Gabriel M. Veith, Dr. Kee Sung Han, Dr. Edward W. Hagaman, Prof. Honglai Liu and Prof. Sheng Dai

      Article first published online: 21 AUG 2012 | DOI: 10.1002/cssc.201200355

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      The art of capturing CO2: A series of porous, nitrogen-doped carbons for CO2 capture have been developed from task-specific ionic liquid (TSIL) precursors by using high-yield carbonization reactions. The porous, nitrogen-doped compound derived from the carbonization of a TSIL exhibits an exceptional CO2 absorption capacity (at 0 °C and 1 bar) because of strong interactions between the CO2 molecules and nitrogen-containing basic sites within the carbon framework.

    4. Amino Acid Ionic Liquid Modified Mesoporous Carbon: A Tailor-made Nanostructure Biosensing Platform (pages 1918–1925)

      Lidong Wu, Xianbo Lu, Haijun Zhang and Jiping Chen

      Article first published online: 20 AUG 2012 | DOI: 10.1002/cssc.201200274

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      Like a mouse in a trap: A novel nanocomposite is obtained by surface modification of graphitized mesoporous carbon (GMC) with hydrophilic and biocompatible amino acid ionic liquids (AAIL). The composite possesses a favorable microenvironment for entrapped tyrosinase, and the GMC–AAIL-based biosensors display superior signal-to-noise ratio and working life.

    5. Photocatalytic and Photoelectrochemical Water Oxidation over Metal-Doped Monoclinic BiVO4 Photoanodes (pages 1926–1934)

      Dr. Kanak Pal Singh Parmar, Hyun Joon Kang, Amita Bist, Dr. Piyush Dua, Dr. Jum Suk Jang and Prof. Jae Sung Lee

      Article first published online: 27 AUG 2012 | DOI: 10.1002/cssc.201200254

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      Performance-enhancing dopants: The photocatalytic and photoelectrochemical water oxidation performance of monoclinic BiVO4 is dramatically enhanced by doping Mo or W into V sites by improving the charge-transfer characteristics. Mo doping generates superior n-type conductivity than that of W doping (see picture).

    6. Cellobiose Hydrolysis and Decomposition by Electrochemical Generation of Acid and Hydroxyl Radicals (pages 1935–1943)

      Youngkook Kwon, Steven E. F. Kleijn, Klaas Jan P. Schouten and Prof. Marc T. M. Koper

      Article first published online: 21 AUG 2012 | DOI: 10.1002/cssc.201200250

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      Electrochemical cellobiose hydrolysis: The hydrolysis of cellobiose to glucose and its further decomposition has been studied with electrochemically generated acid (H+) on a Pt electrode and hydroxyl radicals (OH.) generated on a boron-doped diamond (BDD) electrode. The high local acidity with electrochemically generated H+ on the Pt electrode increases the rate of glucose formation, however, the active electrode (PtOx) interacts with glucose and decomposes it further to smaller organic acids.

    7. Bio-oil Deoxygenation by Catalytic Pyrolysis: New Catalysts for the Conversion of Biomass into Densified and Deoxygenated Bio-oil (pages 1944–1957)

      Dr. Aimaro Sanna and Dr. John M. Andrésen

      Article first published online: 16 AUG 2012 | DOI: 10.1002/cssc.201200245

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      Grains of truth: Catalytic pyrolysis is able to produce bio-oil with a low O and N content and high levels of aliphatics and H from spent grains by using activated serpentine and olivine at 430–460 °C. The biomass oxygenated vapours and aerosols interact in the macro- and mesoporous active sites with the naturally present metallic species to undergo decarboxylation with the formation of CO2 and C5–C6 O-depleted species.

    8. Synthesis of High-Quality Diesel with Furfural and 2-Methylfuran from Hemicellulose (pages 1958–1966)

      Guangyi Li, Dr. Ning Li, Zhiqiang Wang, Dr. Changzhi Li, Prof. Aiqin Wang, Prof. Xiaodong Wang, Prof. Yu Cong and Prof. Tao Zhang

      Article first published online: 21 AUG 2012 | DOI: 10.1002/cssc.201200228

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      Furfural for all: High-quality diesel is obtained from hemicellulose-derived furfural and 2-methylfuran in a satisfactory yield by the combination of hydroxyalkylation–alkylation and hydrodeoxygenation technologies.

    9. Carbon Dioxide Insertion into Diamines: A Computational Study of Solvent Effects (pages 1967–1973)

      Dr. Wilhelm A. Eger, Dr. Alexander Genest, Prof. Dr. Bernhard Rieger and Prof. Dr. Notker Rösch

      Article first published online: 2 OCT 2012 | DOI: 10.1002/cssc.201200222

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      CO2 utilization: In the combined insertion and condensation of CO2 into diamines to yield cyclic ureas, activation barriers, EA, are affected by two properties of the reaction mixture: solvent proton shuttling and moderately increasing the dielectric constant (DC) of the reaction mixture. Separating the two functions of the solvent offers a broad range of tuning options.

    10. One-Step Hydrotreatment of Vegetable Oil to Produce High Quality Diesel-Range Alkanes (pages 1974–1983)

      Congxin Wang, Prof. Zhijian Tian, Dr. Lei Wang, Dr. Renshun Xu, Qianhe Liu, Wei Qu, Dr. Huaijun Ma and Dr. Bingchun Wang

      Article first published online: 4 JUL 2012 | DOI: 10.1002/cssc.201200219

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      From vegetable oil to diesel: The one-step hydrotreatment of vegetable oil combining deoxygenation and isomerization provides a new strategy to directly produce low cloud point, high quality diesel from biomass feedstock. The support acidity of the Pt/zeolite bifunctional catalyst greatly influences this process. Over the catalyst with more Brønsted acid sites and less strong Lewis acid sites, a more economically attractive pathway occurs.

    11. Selective Conversion of Furfural to Maleic Anhydride and Furan with VOx/Al2O3 Catalysts (pages 1984–1990)

      Noelia Alonso-Fagúndez, Dr. Manuel López Granados, Dr. Rafael Mariscal and Dr. Manuel Ojeda

      Article first published online: 30 JUL 2012 | DOI: 10.1002/cssc.201200167

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      Toward future biorefineries: We demonstrate here a promising route to convert renewable furfural to maleic anhydride (max. 73 % yield) and furan (max. 9 % yield) through selective gas-phase oxidation with O2 by using VOx/Al2O3 (0–25 atV nm−2) as solid catalysts. This alternative catalytic technology allows the use of biomass instead of petroleum to synthesize these important chemicals for industry.

    12. Production of Biobutanediols by the Hydrogenolysis of Erythritol (pages 1991–1999)

      Yasushi Amada, Hideo Watanabe, Yuichirou Hirai, Yasuteru Kajikawa, Yoshinao Nakagawa and Keiichi Tomishige

      Article first published online: 3 AUG 2012 | DOI: 10.1002/cssc.201200121

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      Happy hydrogenolysis: The direct hydrogenolysis of erythritol over an Ir–ReOx/SiO2 catalyst is very effective for the production of biobutanediols. The selectivity to butanediols reached 48.0 % at 74.2 % conversion. Based on the production of erythritol by the fermentation of glucose and glycerol, erythritol hydrogenolysis will be promising in the production of biobutanediols.

    13. STEP Wastewater Treatment: A Solar Thermal Electrochemical Process for Pollutant Oxidation (pages 2000–2010)

      Prof. Baohui Wang, Prof. Hongjun Wu, Guoxue Zhang and Prof. Stuart Licht

      Article first published online: 10 SEP 2012 | DOI: 10.1002/cssc.201200305

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      Single STEP: A sustainable methodology of wastewater treatment is presented based on the generalized solar thermal electrochemical production (STEP) process for the conversion and use of solar energy. The STEP process utilizes long-wavelength solar radiation to heat the electrochemical cell, thereby improving both the thermodynamics and kinetics for photovoltaic-driven oxidation. As a proof of concept, the STEP process was utilized to oxidize and remove phenol as a contaminant from artificial wastewater.

    14. Controlling the Adsorption Enthalpy of CO2 in Zeolites by Framework Topology and Composition (pages 2011–2022)

      Lukáš Grajciar, Prof. Jiří Čejka, Dr. Arnošt Zukal, Prof. Carlos Otero Areán, Gemma Turnes Palomino and Prof. Petr Nachtigall

      Article first published online: 10 AUG 2012 | DOI: 10.1002/cssc.201200270

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      Adsorb or not adsorb? The role of different factors that determine the gas–solid interaction energy, such as zeolite topology and zeolite chemical composition, is analyzed based on a combination of accurate ab initio descriptions of CO2 interactions with zeolites and experimental investigations of adsorption heats (see scheme).

    15. Phase Transition of a Cobalt-Free Perovskite as a High-Performance Cathode for Intermediate-Temperature Solid Oxide Fuel Cells (pages 2023–2031)

      Shanshan Jiang, Dr. Wei Zhou, Yingjie Niu, Prof. Zhonghua Zhu and Prof. Zongping Shao

      Article first published online: 27 AUG 2012 | DOI: 10.1002/cssc.201200264

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      Cobalt's denied success: A cobalt-free perovskite (SrNb0.1Fe0.9O3−δ, SNF) shows a phase transition, which is accompanied by a moderate change in the volume, allowing a good cathode/electrolyte interface on thermal cycling. According to the electrochemical impedance spectroscopy evaluation, the I4/m phase of the SNF exhibits positive effects on the cathode's performance, showing the highest oxygen-reduction-reaction activity in cobalt-free cathodes so far.

    16. Merging Sustainability with Organocatalysis in the Formation of Organic Carbonates by Using CO2 as a Feedstock (pages 2032–2038)

      Dr. Christopher J. Whiteoak, Dr. Ainara Nova, Prof. Dr. Feliu Maseras and Prof. Dr. Arjan W. Kleij

      Article first published online: 4 SEP 2012 | DOI: 10.1002/cssc.201200255

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      In a fix: A new organocatalytic method for organic carbonate synthesis is reported and allows attractive conditions (25 °C, 10 bar, no solvent) to be used (see picture). Cyclic carbonates produced from CO2 and epoxides are isolated in high yields. The mild nature of this process increases the overall process sustainability for this type of widely studied carbon dioxide fixation process.

    17. An Efficient and Convenient Palladium Catalyst System for the Synthesis of Amines from Allylic Alcohols (pages 2039–2044)

      Dr. Debasis Banerjee, Dr. Rajenahally V. Jagadeesh, Dr. Kathrin Junge, Dr. Henrik Junge and Prof. Dr. Matthias Beller

      Article first published online: 14 AUG 2012 | DOI: 10.1002/cssc.201200247

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      One pot is all it takes: By applying a convenient combination consisting of Pd(OAc)2/1,10-phenanthroline, a variety of allylic alcohols reacts smoothly to give the corresponding secondary and tertiary amines in good to excellent yields with high regioselectivity (see picture).

    18. Electron-Rich Anthracene Semiconductors Containing Triarylamine for Solution-Processed Small-Molecule Organic Solar Cells (pages 2045–2052)

      Hyeju Choi, Haye Min Ko, Nara Cho, Prof. Kihyung Song, Prof. Jae Kwan Lee and Prof. Jaejung Ko

      Article first published online: 7 AUG 2012 | DOI: 10.1002/cssc.201200242

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      Digging deeper: New electron-rich anthracene derivatives containing a triarylamine hole stabilizer, TIPSAntBT–TPA and TIPSAntBT–bisDMFA, exhibit superior intramolecular charge-transfer performance, resulting in a boost in hole-transporting properties (see picture).

    19. Controlling Surface Enrichment in Polymeric Hole Extraction Layers to Achieve High-Efficiency Organic Photovoltaic Cells (pages 2053–2057)

      Dong-Hun Kim, Kyung-Geun Lim, Prof. Jong Hyeok Park and Prof. Tae-Woo Lee

      Article first published online: 3 SEP 2012 | DOI: 10.1002/cssc.201200202

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      Top job: Hole extraction in organic photovoltaic cells (OPVs) is modulated by a surface-enriched layer formed on top of the conducting polymer-based hole extraction layer (HEL). This tunes the surface work function of the HEL to better align with the ionization potential of the polymeric photoactive layer. Herein, we show a noticeable improvement in device power conversion efficiencies (PCEs) based on rational pretreatment.

    20. Role of Amine Structure on Carbon Dioxide Adsorption from Ultradilute Gas Streams such as Ambient Air (pages 2058–2064)

      Stephanie A. Didas, Ambarish R. Kulkarni, Prof. David S. Sholl and Prof. Christopher W. Jones

      Article first published online: 4 JUL 2012 | DOI: 10.1002/cssc.201200196

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      Out of thin air: The carbon dioxide and water adsorption properties of primary, secondary, and tertiary amine materials are evaluated for the purposes of determining a practical air-capture adsorbent. The amines are ligated to a mesoporous silica support via a propyl linker. The study reveals that the rational design of amine adsorbents for the extraction of carbon dioxide from ambient air should focus on adsorbents rich in primary amines.

    21. Quasi-Homogeneous Oxidation of Glycerol by Unsupported Gold Nanoparticles in the Liquid Phase (pages 2065–2078)

      Dr. Elżbieta Skrzyńska, Jamal Ftouni, Dr. Jean-Sébastien Girardon, Dr. Mickaël Capron, Dr. Louise Jalowiecki-Duhamel, Prof. Jean-François Paul and Prof. Franck Dumeignil

      Article first published online: 7 AUG 2012 | DOI: 10.1002/cssc.201200173

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      Getting the balance right: The product distribution observed during the liquid-phase partial oxidation reaction of glycerol is discussed in terms of balance between reactions specifically induced by the presence of a base in the medium and reactions as a result of the specific action of gold nanoparticles as catalyst (see figure). A global reaction scheme supported by a set of mechanistic analyses is proposed.

    22. Lithium–Sulfur Batteries Based on Nitrogen-Doped Carbon and an Ionic-Liquid Electrolyte (pages 2079–2085)

      Dr. Xiao-Guang Sun, Dr. Xiqing Wang, Dr. Richard T. Mayes and Prof. Sheng Dai

      Article first published online: 30 JUL 2012 | DOI: 10.1002/cssc.201200101

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      NC vs. AC: Nitrogen-doped mesoporous carbon (NC) is prepared by heat treatment of mesoporous carbon under NH3 at 850 °C. Compared with KOH-activated mesoporous carbon (AC), NC shows catalytic activity towards sulfur reduction. Furthermore, under the same current rates, NC/S composite shows a higher discharge potential and capacity than the AC/S composite in an ionic-liquid electrolyte both at 25 °C and 50 °C.

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      Preview: ChemSusChem 11/2012 (page 2087)

      Article first published online: 15 OCT 2012 | DOI: 10.1002/cssc.201290045

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