ChemSusChem

Cover image for Vol. 6 Issue 7

July 2013

Volume 6, Issue 7

Pages 1113–1287

  1. Cover Picture

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    3. Cover Profile
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    6. Masthead
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      Cover Picture: Overcoming Bottlenecks of Enzymatic Biofuel Cell Cathodes: Crude Fungal Culture Supernatant Can Help to Extend Lifetime and Reduce Cost (ChemSusChem 7/2013) (page 1113)

      Sabine Sané, Prof. Dr. Claude Jolivalt, Dr. Gerhard Mittler, Dr. Peter J. Nielsen, Stefanie Rubenwolf, Prof. Dr. Roland Zengerle and Dr. Sven Kerzenmacher

      Version of Record online: 4 JUL 2013 | DOI: 10.1002/cssc.201300547

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      The cover image shows the wood-degrading fungus Trametes versicolor that naturally secretes the redox-enzyme laccase. Without further enzyme purification, the laccase-containing culture supernatant can be supplied to an enzymatic biofuel cell cathode, at which it catalyzes the oxygen reduction reaction. Kerzenmacher et al. show in their manuscript on page 1209 that the enzymes lose catalytic activity with time; for this reason, fresh culture supernatant is regularly resupplied to the electrode to replace the deactivated laccase enzymes. In this way, a comparably simple and cost-efficient enzymatic biofuel cell cathode with an extended lifetime can be established.

  2. Cover Profile

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      Overcoming Bottlenecks of Enzymatic Biofuel Cell Cathodes: Crude Fungal Culture Supernatant Can Help to Extend Lifetime and Reduce Cost (page 1114)

      Sabine Sané, Prof. Dr. Claude Jolivalt, Dr. Gerhard Mittler, Dr. Peter J. Nielsen, Stefanie Rubenwolf, Prof. Dr. Roland Zengerle and Dr. Sven Kerzenmacher

      Version of Record online: 5 JUL 2013 | DOI: 10.1002/cssc.201300520

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      “We can show that the culture supernatant of the enzyme-secreting fungus Trametes versicolor can be used to resupply fresh enzymes at the electrode.” This and more about the story behind the front cover research can be found on page 1209. The front cover can be found on page 1113).

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      Back Cover: Magnetism in Lithium–Oxygen Discharge Product (ChemSusChem 7/2013) (page 1288)

      Dr. Jun Lu, Dr. Hun-Ji Jung, Dr. Kah Chun Lau, Dr. Zhengcheng Zhang, Dr. John A. Schlueter, Dr. Peng Du, Dr. Rajeev S. Assary, Prof. Jeffrey Greeley, Dr. Glen A. Ferguson, Dr. Hsien-Hau Wang, Dr. Jusef Hassoun, Dr. Hakim Iddir, Dr. Jigang Zhou, Dr. Lucia Zuin, Dr. Yongfeng Hu, Prof. Yang-Kook Sun, Prof. Bruno Scrosati, Dr. Larry A. Curtiss and Dr. Kahlil Amine

      Version of Record online: 4 JUL 2013 | DOI: 10.1002/cssc.201300562

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      The Back Cover Image shows an illustration of lithium peroxide nanoparticles growing on a carbon surface. These nanoparticles, reported by Curtiss et al. in their publication on page 1196 show an electronic spin density on the nanoparticle that has been revealed by a combination of experiment and theory. Dr. Hakim Iddir, Dr. Kah Chun Lau, and John Russell contributed considerably to the preparation of this image.

  4. Graphical Abstract

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  5. Masthead

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    1. Masthead: ChemSusChem 7/2013 (page 1125)

      Version of Record online: 5 JUL 2013 | DOI: 10.1002/cssc.201390028

  6. News

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  7. Review

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    1. CaO-Based CO2 Sorbents: From Fundamentals to the Development of New, Highly Effective Materials (pages 1130–1148)

      Dr. Agnieszka M. Kierzkowska, Dr. Roberta Pacciani and Prof. Christoph R. Müller

      Version of Record online: 2 JUL 2013 | DOI: 10.1002/cssc.201300178

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      Lime is fine: Calcium looping is an emerging CO2 capture technology with the potential to substantially reduce capture costs when compared to amine scrubbing. Herein, the current understanding of fundamental aspects of the cyclic carbonation–calcination reactions of CaO is presented. Furthermore, recent attempts to develop synthetic, CaO-based sorbents that possess higher and cyclically more stable CO2 uptakes than limestone are critically reviewed.

  8. Communications

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    1. Solvent-Free Synthesis of C10 and C11 Branched Alkanes from Furfural and Methyl Isobutyl Ketone (pages 1149–1152)

      Jinfan Yang, Dr. Ning Li, Guangyi Li, Dr. Wentao Wang, Aiqin Wang, Dr. Xiaodong Wang, Dr. Yu Cong and Prof. Tao Zhang

      Version of Record online: 11 JUN 2013 | DOI: 10.1002/cssc.201300318

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      Our best results jet: C10 and C11 branched alkanes, with low freezing points, are synthesized through the aldol condensation of furfural and methyl isobutyl ketone from lignocellulose, which is then followed by hydrodeoxygenation. These jet-fuel-range alkanes are obtained in high overall yields (≈90 %) under solvent-free conditions.

    2. Large-Scale Synthesis of Interconnected Si/SiOx Nanowire Anodes for Rechargeable Lithium-Ion Batteries (pages 1153–1157)

      Seungmin Yoo, Jung-In Lee, Myoungsoo Shin and Prof. Soojin Park

      Version of Record online: 13 JUN 2013 | DOI: 10.1002/cssc.201300316

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      Down to the wire: Three-dimensional interconnected Si-based nanowires are produced through the combination of thermal decomposition of SiO and a metal-catalyzed nanowire growth process. This low-cost and scalable approach provides a promising candidate for high-capacity anodes in lithium-ion batteries.

    3. Production of Dimethylfuran from Hydroxymethylfurfural through Catalytic Transfer Hydrogenation with Ruthenium Supported on Carbon (pages 1158–1162)

      Dr. Jungho Jae, Dr. Weiqing Zheng, Prof. Raul F. Lobo and Prof. Dionisios G. Vlachos

      Version of Record online: 10 JUN 2013 | DOI: 10.1002/cssc.201300288

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      RuC ees′ transfer: Transfer hydrogenation using alcohols as hydrogen donors and supported ruthenium catalysts results in the selective conversion of hydroxymethylfurfural to dimethylfuran (>80 % yield). During transfer hydrogenation, the hydrogen produced from alcohols is utilized in the hydrogenation of hydroxymethylfurfural.

    4. Conversion of Carbohydrate Biomass to γ-Valerolactone by using Water-Soluble and Reusable Iridium Complexes in Acidic Aqueous Media (pages 1163–1167)

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

      Version of Record online: 11 JUN 2013 | DOI: 10.1002/cssc.201300245

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      Mild-mannered manipulation: A catalytic method for the conversion of carbohydrate biomass to γ-valerolactone in acidic aqueous media has been developed. The water-soluble iridium complexes were observed to be extremely catalytically active for providing γ-valerolactone in high yields with high TONs. The homogeneous catalysts can also be recycled and reused by applying a simple phase separation process.

    5. One-step Synthesis and Chemical Characterization of Pt–C Nanowire Composites by Plasma Sputtering (pages 1168–1171)

      Dr. Pascal Brault, Dr. Amaël Caillard, Dr. Stève Baranton, Dr. Matthieu Mougenot, Dr. Stéphane Cuynet and Prof. Christophe Coutanceau

      Version of Record online: 13 JUN 2013 | DOI: 10.1002/cssc.201300236

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      Plasma increases activity: A one-step synthesis of Pt–C nanowire composites using a plasma co-deposition method is reported. Electrodes with a very low Pt loading can be obtained. Pt particles with sizes ranging from 1 to 2 nm are decorating the columnar carbon nanostructures because of strong interactions. The composite microstructure is responsible for a very high metal utilization rate as exemplified by reactions occurring in fuel cell electrodes.

    6. Towards a Practical Setup for Hydrogen Production from Formic Acid (pages 1172–1176)

      Peter Sponholz, Dörthe Mellmann, Dr. Henrik Junge and Prof. Matthias Beller

      Version of Record online: 11 JUN 2013 | DOI: 10.1002/cssc.201300186

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      Formic acid cracker: A mini plant that allows for continuous formic acid decomposition to hydrogen and carbon dioxide under ambient conditions is presented. By using an in situ-formed ruthenium catalyst, unprecedented turnover numbers over 1 000 000 are achieved. The active catalyst is formed in situ from commercially available [RuCl2(benzene)]2 and 1,2-bisdiphenylphosphinoethane.

    7. Li-S Battery Analyzed by UV/Vis in Operando Mode (pages 1177–1181)

      Manu U. M. Patel, Dr. Rezan Demir-Cakan, Dr. Mathieu Morcrette, Prof. Jean-Marie Tarascon, Prof. Miran Gaberscek and Dr. Robert Dominko

      Version of Record online: 7 JUN 2013 | DOI: 10.1002/cssc.201300142

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      Battery watch: UV/Vis spectrophotometry is demonstrated as a powerful analytical method for the in situ study of polysulfides. Through the interactions that occur between different chain-length polysulfide molecules and the UV/Vis radiation, quantitative and qualitative determination of the polysulfides formed during Li–S battery operation can be achieved.

    8. Polyurethanes from Isosorbide-Based Diisocyanates (pages 1182–1185)

      Michael D. Zenner, Dr. Ying Xia, Prof. Dr. Jason S. Chen and Prof. Dr. Michael R. Kessler

      Version of Record online: 11 JUN 2013 | DOI: 10.1002/cssc.201300126

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      Benign building blocks: Stereochemically pure diisocyanates were prepared on a multigram scale from succinic anhydride and isosorbide or isomannide. Characterization of polyurethanes that were produced from these diisocyanates revealed low polydispersity, high thermal stability, and stereochemistry-dependent morphology. If biobased succinic anhydride is used, then no stoichiometric petroleum-derived reagents are required in the synthesis of these materials.

    9. Mesoporous Poly(Melamine–Formaldehyde) Solid Sorbent for Carbon Dioxide Capture (pages 1186–1190)

      Dr. Mei Xuan Tan, Dr. Yugen Zhang and Prof. Jackie Y. Ying

      Version of Record online: 11 JUN 2013 | DOI: 10.1002/cssc.201300107

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      Feed the pore: A highly mesoporous melamine–formaldehyde resin is synthesized through a simple, one-step polycondensation reaction by using inexpensive and abundant common industrial chemicals. The material is demonstrated to have a high surface area and a well-defined pore structure. Its high density of CO2 binding pockets with low CO2 binding energy facilitates rapid and reversible CO2 sorption.

  9. Full Papers

    1. Top of page
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    6. Masthead
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    1. Reversible Capture of SO2 through Functionalized Ionic Liquids (pages 1191–1195)

      Dezhong Yang, Minqiang Hou, Hui Ning, Jun Ma, Xinchen Kang, Jianling Zhang and Prof. Buxing Han

      Version of Record online: 16 MAY 2013 | DOI: 10.1002/cssc.201300224

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      Say it ain′t SO2! The ionic liquid [Et2NEMim][Tetz] is synthesized and demonstrated to have an extremely high absorption capacity and rapid absorption/desorption rates for the capture of SO2. [Et2NEMim][Tetz] can be regenerated and reused, making it a very attractive ionic liquid for practical SO2 capture applications.

    2. Magnetism in Lithium–Oxygen Discharge Product (pages 1196–1202)

      Dr. Jun Lu, Dr. Hun-Ji Jung, Dr. Kah Chun Lau, Dr. Zhengcheng Zhang, Dr. John A. Schlueter, Dr. Peng Du, Dr. Rajeev S. Assary, Prof. Jeffrey Greeley, Dr. Glen A. Ferguson, Dr. Hsien-Hau Wang, Dr. Jusef Hassoun, Dr. Hakim Iddir, Dr. Jigang Zhou, Dr. Lucia Zuin, Dr. Yongfeng Hu, Prof. Yang-Kook Sun, Prof. Bruno Scrosati, Dr. Larry A. Curtiss and Dr. Kahlil Amine

      Version of Record online: 13 MAY 2013 | DOI: 10.1002/cssc.201300223

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      In a spin: The major discharge product formed in the lithium–oxygen cell, lithium peroxide, exhibits a magnetic moment. Density functional calculations predict that “superoxide-like” surface oxygen groups with unpaired electrons exist on nanoparticle surfaces, consistent with magnetic measurements of discharged lithium peroxide products. The “superoxide-like” surface oxygen groups with spin can play a role in the reversible formation and decomposition of lithium peroxide as well as electrolyte molecules.

    3. Controlled Hydrophobic Functionalization of Natural Fibers through Self-Assembly of Amphiphilic Diblock Copolymer Micelles (pages 1203–1208)

      Niko Aarne, Prof. Janne Laine, Dr. Tuomas Hänninen, Ville Rantanen, Dr. Jani Seitsonen, Prof. Janne Ruokolainen and Dr. Eero Kontturi

      Version of Record online: 17 MAY 2013 | DOI: 10.1002/cssc.201300218

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      Rough and ready: A platform technology for the hydrophobization of natural fibers in water through amphiphilic block copolymer micelle adsorption onto fibers and subsequent heating. The natural roughening of the fibers upon drying facilitates hydrophobization, and heating reveals the hydrophobic core, which allows further hydrophobizing of the surface. Heat treatment tunes the effect of changes to the advancing water contact angles of 120° to 150°.

    4. Overcoming Bottlenecks of Enzymatic Biofuel Cell Cathodes: Crude Fungal Culture Supernatant Can Help to Extend Lifetime and Reduce Cost (pages 1209–1215)

      Sabine Sané, Prof. Dr. Claude Jolivalt, Dr. Gerhard Mittler, Dr. Peter J. Nielsen, Stefanie Rubenwolf, Prof. Dr. Roland Zengerle and Dr. Sven Kerzenmacher

      Version of Record online: 25 JUN 2013 | DOI: 10.1002/cssc.201300205

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      Using microorganisms for enzymatic biofuel cells: Enzymes in crude culture supernatant of the fungus Trametes versicolor are used at an enzymatic biofuel cell cathode without further purification. The lifetime of an enzymatic cathode can be extended by resupplying fresh enzymes from the crude culture supernatant. This can enable the development of a simple, mediatorless, and cost-efficient enzymatic biofuel cell cathode with an extended lifetime.

    5. Polyethyleneimine-Functionalized Polyamide Imide (Torlon) Hollow-Fiber Sorbents for Post-Combustion CO2 Capture (pages 1216–1223)

      Fuyue Stephanie Li, Dr. Wulin Qiu, Dr. Ryan P. Lively, Dr. Jong Suk Lee, Dr. Ali A. Rownaghi and Prof. William J. Koros

      Version of Record online: 24 MAY 2013 | DOI: 10.1002/cssc.201300172

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      Sucked in! Polyethyleneimine (PEI)-functionalized polymeric hollow-fiber sorbents for post-combustion carbon dioxide capture are described. Different molecular weight PEIs are studied as functional groups on polyamide imide (PAI) hollow fibers. For equivalent PEI concentrations, PAI functionalized with lower molecular weight PEI exhibit higher CO2 capacities (see picture).

    6. Preparation of Glycerol Carbonate Esters by using Hybrid Nafion–Silica Catalyst (pages 1224–1234)

      Prof. Dr. María J. Climent, Prof. Dr. Avelino Corma, Prof. Dr. Sara Iborra, Sergio Martínez-Silvestre and Dr. Alexandra Velty

      Version of Record online: 10 JUN 2013 | DOI: 10.1002/cssc.201300146

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      Chain reaction: The esterification of glycerol carbonate with carboxylic acids to produce glycerol carbonate esters, which are valuable biomass-derivative compounds, has been investigated. A Nafion–silica nanocomposite is shown to be an excellent catalyst, and after fitting the experimental data to a kinetic model, the kinetic parameters were determined and compared for reactions involving different carboxylic acids.

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      Methane Adsorption on Aggregates of Fullerenes: Site-Selective Storage Capacities and Adsorption Energies (pages 1235–1244)

      Alexander Kaiser, Samuel Zöttl, Dr. Peter Bartl, Dr. Christian Leidlmair, Dr. Andreas Mauracher, Prof. Dr. Michael Probst, Dr. Stephan Denifl, Prof. Dr. Olof Echt and Prof. Dr. Paul Scheier

      Version of Record online: 6 JUN 2013 | DOI: 10.1002/cssc.201300133

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      Snuggling of bucky and methane: What are the preferred adsorption sites of methane on small aggregates of C60? How many methane molecules adsorb in groove sites? How many in dimple sites? We provide answers for aggregates containing up to four C60 molecules. For example, this figure shows that seven CH4 fit into the groove of the dimer, in excellent agreement with experiment. Calculated adsorption energies of 118–281 meV are in the optimal range for high-density storage of natural gas.

    8. Structural Characterization of Anion–Calcium–Humate Complexes in Phosphate-based Fertilizers (pages 1245–1251)

      Dr. Roberto Baigorri, Dr. Oscar Urrutia, Dr. Javier Erro, Dr. Marcos Mandado, Dr. Ignacio Pérez-Juste and Dr. José María Garcia-Mina

      Version of Record online: 13 MAY 2013 | DOI: 10.1002/cssc.201300024

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      Complex fertilizers: The combination of computational chemistry and traditional analysis allows the explanation of unexpected trends in the intensity and fine structure of the peaks obtained through 31P NMR spectroscopy for phosphate-based fertilizers. A sulfate–calcium-humate complex is predicted and confirmed, which has not previously been reported.

    9. Microscale Gradients of Oxygen, Hydrogen Peroxide, and pH in Freshwater Cathodic Biofilms (pages 1252–1261)

      Dr. Jerome T. Babauta, Dr. Hung Duc Nguyen, Dr. Ozlem Istanbullu and Dr. Haluk Beyenal

      Version of Record online: 13 JUN 2013 | DOI: 10.1002/cssc.201300019

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      A river runs through: Sediment microbial fuel cells are a new technology used to harness the natural redox gradients in sediments to produce usable energy. Microbial catalysis of oxygen reduction is often used to enhance the recovery of energy by sediment microbial fuel cells. It is demonstrated that microscale gradients of pH, oxygen, and hydrogen peroxide resulting from oxygen reduction negatively affects the colonization of micro-organisms on cathode surfaces that could be used in sediment microbial fuel cells.

    10. Morphology and Electrochemical Properties of Perfluorosulfonic Acid Ionomers for Vanadium Flow Battery Applications: Effect of Side-Chain Length (pages 1262–1269)

      Cong Ding, Prof. Huamin Zhang, Prof. Xianfeng Li, Hongzhang Zhang, Chuan Yao and Dingqin Shi

      Version of Record online: 14 JUN 2013 | DOI: 10.1002/cssc.201300014

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      Membrane fame! A membrane with short side chains is proposed for vanadium flow batteries for the first time. This membrane (Aquivion-E87-12S) displays a much lower degree of hydrophobic–hydrophilic separation and exhibits superior coulombic efficiency than Nafion along with a remarkable capacity retention.

    11. Degradation of Cyanoacrylic Acid-Based Organic Sensitizers in Dye-Sensitized Solar Cells (pages 1270–1275)

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

      Version of Record online: 14 JUN 2013 | DOI: 10.1002/cssc.201200949

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      Dye-ing to degrade: The degradation mechanism of cyanoacrylic acid-based organic sensitizers in dye-sensitized solar cells (DSSCs) has been studied. With the synergy of water and UV light, the sensitizer desorbs from the TiO2 surface and the cyanoacrylic acid unit of sensitizer is converted into an aldehyde group. It is also observed that the oxygen atom of the aldehyde comes from the solvent water in DSSCs.

    12. Self-Biasing Photoelectrochemical Cell for Spontaneous Overall Water Splitting under Visible-Light Illumination (pages 1276–1281)

      Dr. Quanpeng Chen, Dr. Jinhua Li, Dr. Xuejin Li, Dr. Ke Huang, Prof. Dr. Baoxue Zhou and Prof. Wenfeng Shangguan

      Version of Record online: 17 JUN 2013 | DOI: 10.1002/cssc.201200936

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      WO3/W—wow! A self-biasing photoelectrochemical cell based on a Pt-catalyst-decorated crystalline silicon photovoltaic cell photocathode and WO3/W photoanode that can be self-driven for overall water splitting under visible-light illumination is described.

    13. Amorphous Cu–In–S Nanoparticles as Precursors for CuInSe2 Thin-Film Solar Cells with a High Efficiency (pages 1282–1287)

      Dr. SeJin Ahn, Yoo Jeong Choi, Kyunhwan Kim, Dr. Young-Joo Eo, Ara Cho, Dr. Jihye Gwak, Dr. Jae Ho Yun, Dr. Keeshik Shin, Dr. Seoung Kyu Ahn and Dr. Kyunghoon Yoon

      Version of Record online: 16 MAY 2013 | DOI: 10.1002/cssc.201200894

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      CuInS a phase: An amorphous Cu–In–S nanoparticle-based route to form dense CuInSe2 absorber layers for thin-film solar cells, in which the precursor nanoparticles are prepared within one minute of reaction without external heating, is demonstrated. A power conversion efficiency as high as 7.94 % is achieved by using this method.

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