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Changwei Hu, Zhicheng Jiang, Pingping Zhao, Jianmei Li, Xudong Liu
The dissolution of cellulose from biomass is a crucial but complicated issue for the utilisation of biomass resources, because of the extreme insolubility of cellulose. Herein, a biphasic NaCl-H2O-tetrahydrofuran system was studied, where most of the pure microcrystalline cellulose (M-cellulose, 96.6% conversion at 220 oC) and that contained in actual biomass were converted. Nearly a half of O(6)H***O(3) intermolecular hydrogen bonding could be broken by THF in H2O-THF co-solvent system, whereas the cleavage of O(2)H***O(6) intramolecular hydrogen bonding by H2O was significantly inhibited...
November 17, 2017: ChemSusChem
Avelino Corma, Pilar García-García, Sergio Rojas-Buzo
A series of highly crystalline, porous, hafnium-based metal-organic frameworks (MOFs) have shown to catalyze the transfer hydrogenation reaction of levulinic ester to produce γ-valerolactone using isopropanol as hydrogen donor and the results are compared with the zirconium-based counterparts. The role of the metal center in Hf-MOFs has been identified and reaction parameters optimized. NMR studies with isotopically labeled isopropanol evidences that the transfer hydrogenation occurs via a direct intermolecular hydrogen transfer route...
November 15, 2017: ChemSusChem
Hongliang Wang, Huamin Wang, Eric Kuhn, Melvin P Tucker, Bin Yang
Super Lewis acids containing the triflate anion [e.g., Hf(OTf)4 , Ln(OTf)3 , In(OTf)3 , Al(OTf)3 ] and noble metal catalysts (e.g., Ru/C, Ru/Al2 O3 ) formed efficient catalytic systems to generate saturated hydrocarbons from lignin in high yields. In such catalytic systems, the metal triflates mediated rapid ether bond cleavage through selective bonding to etheric oxygens while the noble metal catalyzed subsequent hydrodeoxygenation (HDO) reactions. Near theoretical yields of hydrocarbons were produced from lignin model compounds by the combined catalysis of Hf(OTf)4 and ruthenium-based catalysts...
November 14, 2017: ChemSusChem
Cristina Flox, Sebastián Murcia-López, Nina M Carretero, Carles Ros, Juan Ramón Morante, Teresa Andreu
The ability of crystalline Si to photo-assist the V3+/V2+ cathodic reaction under simulated solar irradiation, combined with the effect of Bi have led to important electrochemical improvements. Besides the photo-voltage supplied by the photovoltaics, additional decrease in the onset potentials, high reversibility of the V3+/V2+ redox pair and improvement in the electro-kinetics have been attained thanks to the addition of Bi. In fact, Bi0 deposition has shown to slightly decrease the photocurrent, but the significant betterment in the charge transfer, reflected in the overall electrochemical performance clearly justifies its use as additive in a photo-assisted system for maximizing the efficiency of solar charge to battery...
November 14, 2017: ChemSusChem
Holger Dau, Etsuko Fujita, Licheng Sun
In this Editorial, Guest Editors Holger Dau, Etsuko Fujita, and Licheng Sun introduce the Special Issue of ChemSusChem on "Artificial Photosynthesis for Sustainable Fuels". They discuss the need for non-fossil based fuels, introduce both biological and artificial photosynthesis, and outline various important concepts in artificial photosynthesis, including molecular and solid-state catalysts for water oxidation and hydrogen evolution, catalytic CO2 reduction, and photoelectrochemical systems.
November 13, 2017: ChemSusChem
Priyadharsini Karuppuswamy, Hung-Cheng Chen, Pen-Cheng Wang, Chao-Ping Hsu, Ken-Tsung Wong, Chih Wei Chu
In this work, we introduced benzo[ghi]perylenetriimide (BPTI) derivatives including monomer and twisted dimer (t-BPTI) as an alternative electron transport layer (ETL) material to replace the commonly used PC61BM in inverted planar heterojunction perovskite solar cells. Moreover, the double ETL layer was applied in our perovskite solar cells with structure of glass/ITO/PEDOT:PSS/perovskite/BPTI/C60 or PDI-C4/BCP/Al. Use of a double ETL layer structure can effectively eliminate the leakage current. The devices with the t-BPTI/C60 double ETL layer yield an average power conversion efficiency of 10...
November 12, 2017: ChemSusChem
Shaowei Chen, Yi Peng, Wanzhang Pan, Nan Wang, Jia-En Lu
Carbon-based materials are promising, low-cost electrocatalysts toward hydrogen evolution reaction (HER), although the catalytic performance needs to be further improved before commercialization. In this study, ruthenium ions are incorporated into carbon nitride-reduced graphene oxide hybrids forming C3N4-rGO-Ru composites through RuN coordination. The incorporation of Ru ions, at a loading of 1.93 at.%, leads to electron redistribution within the materials and dramatically enhances the HER performance, as compared to C3N4, C3N4-rGO, and C3N4-Ru, with an overpotential of only 80 mV to reach the current density of 10 mA/cm2, a Tafel slope of 55 mV/dec, and an exchange current density of 0...
November 9, 2017: ChemSusChem
Shuang Cao, Chuan-Jun Wang, Wen-Fu Fu, Yong Chen
Solar-to-hydrogen conversion based on photocatalytic and photoelectrocatalytic water splitting is considered as a promising technology for sustainable hydrogen production. Developing earth-abundant H2 -production materials with robust activity and stability has become the mainstream in this field. Due to the unique properties and characteristics, transition metal phosphides (TMPs) have been proven to be high performance co-catalysts to replace some of the classic precious metal materials in photocatalytic water splitting...
November 9, 2017: ChemSusChem
Paola Lanzafame, Salvatare Abate, Claudio Ampelli, Chiara Genovese, Rosalba Passalacqua, Gabriele Centi, Siglinda Perathoner
The future feasibility of decarbonized industrial chemical production based on the substitution of fossil feedstocks (FFs) with renewable energy (RE) sources is discussed. Indeed, the use of FFs as an energy source has the greatest impact on the greenhouse gas emissions of chemical production. This future scenario is indicated as "solar-driven" or "RE-driven" chemistry. Its possible implementation requires to go beyond the concept of solar fuels, in particular to address two key aspects: i) the use of RE-driven processes for the production of base raw materials, such as olefins, methanol, and ammonia, and ii) the development of novel RE-driven routes that simultaneously realize process and energy intensification, particularly in the direction of a significant reduction of the number of the process steps...
November 9, 2017: ChemSusChem
Wenjun Du, Lingyao Li, Sampa Maiti, Nicole A Thompson, Lan J Miligan
The capability of a polymer to depolymerize, which regenerates its original monomer for further polymerization, is very attractive in terms of sustainability. Sugar poly(orthoester) was recently synthesized as a novel class of glycopolymer. The high sensitivity of the backbone orthoester linkage towards acidolysis provides a valuable model to study its depolymerization. Herein, we report that the sugar poly(orthoester) can be completely depolymerized at slightly acidic conditions. However, in most cases, the depolymerization gave a stable cyclic product (1,6-anhydro glucopyranose), instead of its original monomer...
November 9, 2017: ChemSusChem
Shuang Ma, Ellen van Heeswijk, Bart Noordover, Rafael Sablong, Rolf van Benthem, Cor Koning
In this work, an isocyanate-free approach to produce polyureas from diamines and dicarbamates as monomers is reported. A side reaction limiting molecular weight during the diamine/dicarbamate polymerization, viz. N-alkylation of amine end-groups, is investigated. Mitigation of the N-alkylation, either by enhancing the carbamate aminolysis rate or by substitution of dimethylcarbamates with more sterically hindered diethylcarbamates, affords polyureas with sufficiently high molecular weights to assure satisfactory mechanical properties...
November 8, 2017: ChemSusChem
Nicolas Alonso-Vante, Yun Luo, Björn Kirchhoff, Donato Fantauzzi, Laura Calvillo, Luis Alberto Estudillo-Wong, Gaetano Granozzi, Timo Jacob
Improving the efficiency of Pt-based oxygen reduction reaction (ORR) catalysts while also reducing costs remains an important challenge in energy research. To this end, we synthesized highly stable and active carbon-supported Mo-doped PtCu (Mo-PtCu/C) nanoparticles (NPs) from readily available precursors in a facile one-pot reaction. Mo-PtCu/C displays two- to four-fold higher ORR half-cell kinetics than reference PtCu/C and Pt/C materials - a trend which was confirmed in proof-of-concept experiments using a H2/O2 micro-laminar fuel cell...
November 7, 2017: ChemSusChem
Tiina Laaksonen, Jussi Kari Juhani Helminen, Laura Lemetti, Jesper Långbacka, Daniel Rico Del Cerro, Michael Hummel, Erkko Ilari Filpponen, Antti Rantamäki, Tia Kakko, Marianna Kemell, Susanne Wiedmer, Sami Heikkinen, Ilkka Kilpeläinen, Alistair William Thomas King
It is shown that ionic liquids can be used to dewater birch kraft pulp cellulose nanofibrillar (CNF) suspension and act as a medium for water-free topochemical modification of the nanocellulose. Acetylation, was applied as a model reaction to investigate the degree of modification and scope of effective ionic liquid structures. Little difference in reactivity was observed when water was removed, after introduction of ionic liquid or molecular co-solvent. However, the viscoelastic properties of CNF suspended in two ionic liquids showed that the more basic, but non-dissolving ionic liquid, allows for better solvation of the CNF...
November 7, 2017: ChemSusChem
Ahmad Arabi Shamsabadi, Farzad Seidi, Mohammad Nozari, Masoud Soroush
In addition to possessing excellent chemical, mechanical and thermal stability, polyimides and polyetherimides have excellent solubility in many solvents, rendering them suitable for membrane preparation. In this paper, we report the synthesis and characterization of two new monomers [a pentiptycene-based dianhydride (PPDAn) and a pentiptycene imide-containing diamine (PPImDA)], and a pentiptycene-based polyimide [PPImDA-4, 4'-hexafluoroisopropylidene diphthalic anhydride (PPImDA-6FDA)]. The products are characterized using FTIR, 1H NMR, GPC, mass spectroscopy, XPS, TGA, DSC, BET, and XRD...
November 6, 2017: ChemSusChem
Dong Un Lee, Moon Gyu Park, Zachary Paul Cano, Wook Ahn, Zhongwei Chen
Nano-engineered hierarchical core-shell chestnut-like structures have been successfully synthesized as a bi-functionally active electrocatalyst for rechargeable metal-air battery applications. Both the morphology and composition of the catalyst have been optimized by the facile hydrothermal reaction, resulting in the 10-hour treated sample to perform significantly enhanced activity towards facilitating both oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). Specifically, the catalyst demonstrated -0...
November 5, 2017: ChemSusChem
Qiang Guo, Li Chen, Zizhao Shan, Wee Siang Vincent Lee, Wen Xiao, Zhifang Liu, Jingjing Liang, Gaoli Yang, Junmin Xue
H2Ti12O25 holds great promise as high voltage anode material for advanced lithium-ion battery application. In order to enhance its electrochemical performance, controlling crystal orientation and morphology is one of the effective ways to cope the slow Li+ diffusion inside H2Ti12O25 with severe anisotropy. In this report, Na2Ti6O13 nanorods, prepared with Na2CO3 and anatase TiO2 in molten NaCl medium, were used as a precursor in the synthesis of long single-crystal H2Ti12O25 nanorods with reactive facets. As-prepared H2Ti12O25 nanorods with the diameter of 100-200 nm show higher charge (extraction) specific capacity and better rate performance as compared to the previously reported system...
November 4, 2017: ChemSusChem
Yuxing Xu, Ailong Li, Tingting Yao, Changtong Ma, Xianwen Zhang, Jafar Hussain Shah, Hongxian Han
Converting sunlight to solar fuels by artificial photosynthesis is an innovative science and technology for renewable energy. Light harvesting (LH), photogenerated charge separation and transfer (CST), and catalytic reactions (CR) are the three primary steps in the processes of solar energy to chemical energy (SE-CE) conversion. Among them, the CST is the key "energy pump and delivery" step in determining the overall solar energy conversion efficiency. Efficient CST is always the priority concern in designing and assembling artificial photosynthesis systems for solar fuels production...
November 4, 2017: ChemSusChem
Xiao-Yu Wu, Ahmed F Ghoniem
Kinetics data for CO2 thermochemical reduction in an isothermal membrane reactor is required to identify the rate-limiting steps. Here, we report a detailed reaction kinetics study on this process supported by an La0.9Ca0.1FeO3-δ (LCF-91) membrane. The dependence of CO2 reduction rate on various operating conditions is examined such as CO2 concentration on the feed side, fuel concentrations on the sweep side and temperatures. CO2 reduction rate is proportional to the oxygen flux across the membrane, and the measured maximum fluxes are 0...
November 4, 2017: ChemSusChem
Aura Tolosa, Simon Fleischmann, Ingrid Grobelsek, Antje Quade, Eunho Lim, Volker Presser
This study introduces the synthesis of free-standing, binder-free, titanium-niobium oxide/carbon hybrid nanofibers for Li-ion battery applications. The one-pot synthesis offers a significant reduction of processing steps and avoids the use of environmentally unfriendly binder materials, making the approach highly sustainable. Tetragonal Nb2O5/C and monoclinic Ti2Nb10O29/C hybrid nanofibers synthesized at 1000 °C presented the highest electrochemical performance, with capacity values of 243 and 267 mAh∙g-1, respectively normalized to the electrode mass...
November 3, 2017: ChemSusChem
Kwiyong Kim, Seung Jong Lee, Dong-Yeon Kim, Chung-Yul Yoo, Jang Wook Choi, Jong-Nam Kim, Youngmin Woo, Hyung Chul Yoon, Jong-In Han
Lithium-mediated reduction of dinitrogen is a promising way to evade electron-stealing hydrogen evolution, a critical challenge which limits faradaic efficiency (FE) and thus hinders the success of traditional protic solvent-based ammonia electro-synthesis. In this study, we propose a viable illustration to realize the lithium-mediated pathway using lithium-ion conducting glass ceramic, which can be divided into three successive steps: (i) lithium deposition, (ii) nitridation, and (iii) ammonia formation. Ammonia was successfully synthesized from molecular nitrogen and water, yielding a maximum FE of 52...
November 3, 2017: ChemSusChem
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