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Andreas Gansäuer, Theresa Liedtke, Tobias Hilche, Sven Klare
Our cyclic voltammetry-based screening method for Cp2TiX-catalyzed reactions is extended to the screening of other solvents for bulk electrolysis of the catalyst and radical arylation. It was found that CH3CN is a solvent that can be used for both processes without additives. Furthermore, in THF, squaramide L2 is more efficient than our previously best supramolecular halide binder, Schreiner's thiourea L1. The results extend the usefulness of our time and resource efficient screening method for the reaction design in catalysis in single-electron steps...
February 19, 2019: ChemSusChem
Shahzada Ahmad, Manuel Salado, Samrana Kazim, Mohammad Khaja Nazeeruddin
Three-dimensional hybrid perovskite materials (CH3NH3PbI3) suffer from intrinsic instability due to organic cation evaporation and ion migration. The inclusion of a large organic cation such as guanidinium has been probed to stabilize the structure. In this work, we put forward the inclusion of imidazolium iodide (C3N2H5I) as organic cation inside the CH3NH3PbI3 matrix, as a reservoir to control the spontaneous loss of iodide. The introduction of imidazolium iodide in amounts below 20% has an impact on the crystallization process but not on the optical properties, and positively controls non-radiative recombination and allows to improve the open circuit voltage of the solar cells...
February 18, 2019: ChemSusChem
Carmine Gaeta, Pellegrino La Manna, Annunziata Soriente, Margherita De Rosa, Antonio Buonerba, Carmen Talotta, Placido Neri
A metal-free Friedel-Crafts benzylation (FCB) of scarcely reactive arenes and heteroarenes has been performed under on-water conditions through an environmentally-sustainable procedure. Our catalytic strategy exploits the hydrophobicity of the resorcinarene macrocycle (1a). The proposed mechanism is based on the activation of benzyl chloride by H-bonding interactions with catalyst 1a. In fact, under on-water conditions the hydrophobic amplification of the strength of the H-bond interactions between the OH groups of the resorcinarene catalyst and the chlorine atom of the benzyl chloride, led to the polarization of the C-Cl bond that consequently promotes the electrophilic attack of the π-nucleophile...
February 18, 2019: ChemSusChem
Yuanxing Fang, Xiaochun Li, Xinchen Wang
Overcoming the sluggish kinetics of the water oxidation is the key to lead a high performance for solar water splitting. Herein, we find that phosphorylated polymeric carbon nitride (PCN) photoanodes present enhanced photocurrent density for solar water splitting, and the photocatalytic efficiency is achieved 120 µA/cm2 in basic solution (1.0 M NaOH) without scarifice agent. In this sytem, phosphates ionically anchor on the surface of PCN, and the modified films show significantly increased density of valance electrons, and thus promoting photoelectrocatalytic efficiency...
February 18, 2019: ChemSusChem
Alain Goeppert, Hang Zhang, Raktim Sen, Huong Dang, Surya G Prakash
Carbon dioxide adsorbents based on the reaction of pentaethylenehaxamine (PEHA) or tetraethylenepentamine (TEPA) with propylene oxide (PO) were easily prepared in "one pot" by impregnation on a silica support in water. The starting materials are readily available and have a low cost facilitating the production of the adsorbents on a large scale. The prepared polyamine/epoxide adsorbents were efficient in capturing CO2 and regenerable under mild conditions (50-85 °C). They displayed a much improved stability compared to their unmodified amine counterparts, especially under oxidative conditions...
February 15, 2019: ChemSusChem
Hiroshi Onishi
Sodium tantalate (NaTaO3) is the first semiconductor photocatalyst which produces hydrogen-oxygen mixed bubbles in the overall water splitting reaction, when properly doped with metal cations. A series of studies are reviewed here to answer the question of why doping with metal cations raised the quantum efficiency of the reaction. Infrared absorption of bandgap-excited photocatalysts demonstrated that cation doping reduced the electron-hole recombination rate and the steady-state population of charge carriers accordingly increased...
February 15, 2019: ChemSusChem
Zhuoran Wang, Hsien-Chieh Chiu, Andrea Paolella, Karim Zaghib, George Demopoulos
Integration of solar energy harvesting and storage functions attracts significant research attention as it holds promise for ultimate development of light-chargeable devices. In this context, we investigate a functional nanocomposite anode that does not only permit electrochemical energy storage via Li-ion photo-intercalation, but also exhibits potential for photoelectrochromic applications. The nanocomposite is made of the Li-ion intercalation compound WO3 (thinly coated with TiO2) and sensitized by the photoactive semicoductor CdS...
February 15, 2019: ChemSusChem
Daniel Mack, Sabrina Schätzle, Yvonne Traa, Elias Klemm
Acrylonitrile (ACN) is widely used as monomer in the synthesis of polymers and carbon fibers. Nowadays, its production is based on fossil resources. Herein, we present an alternative process based on renewable resources. Lactic acid (LA) obtained by fermentation of biomass is converted to ACN in two steps with an overall selectivity of 57%. In the first step, a direct amidation of LA in the presence of water is conducted at 230 °C. Zeolites can catalyze the formation of lactamide, and a selectivity of 92% is reached at 33% conversion with NH4-ZSM-5...
February 15, 2019: ChemSusChem
Longlong Ma, Haiyong Wang, Changhui Zhu, Qiying Liu, Jin Tan, Chenguang Wang, Zheng Liang
Hydroxyacetone (HA) and 1-hydroxy-2-butanone (HB), both of which contain carbonyl and hydroxyl groups, are becoming increasingly important as intermediates,due to their diversified applications in fine chemicals production such as medicine and food additives. We developed astrategyto obtain these two products from direct cellulose conversion over Sn-Ni intermetallic compound (IMC) catalysts. It was confirmed that the Sn-Ni IMC and SnOx acted as the active sitesfor HA and HB production via selectively cleaving the target C-C and C-O bonds...
February 14, 2019: ChemSusChem
Jeannine Mayr, Jan-Hendrick Grosch, Lena Hartmann, Luis F M Rosa, Antje C Spiess, Falk Harnisch
Chiral alcohols constitute important building blocks that can be produced enantioselectively using NAD(P)H-dependent oxidoreductases. For NAD(P)H regeneration, electricity delivers the cheapest reduction equivalents. Enzymatic electrosynthesis suffers from cofactor and enzyme instability, whereas microbial electrosynthesis (MES) exploits whole cells. Here, we demonstrate MES using resting Escherichia coli as biocatalytic chassis for a production platform towards fine chemicals using electric power. This chassis was exemplified for the synthesis of chiral alcohols by using a NADPH-dependent alcohol dehydrogenase from Lactobacillus brevis for synthesis of (R)-1-phenylethanol from acetophenone...
February 14, 2019: ChemSusChem
Zhongqiao Ma, Cheng Lian, Dong Fang Niu, Lei Shi, Shuozhen Hu, Xinsheng Zhang, Honglai Liu
Selective electrochemical reduction of CO2 using renewable electricity has received considerable attention because of the potential to convert a harmful greenhouse gas to a useful chemical. In this report, we construct a high-performance electrocatalyst based on metal nanoparticles/organic molecule hybrid materials for CO2 reduction. On the nanoscale, Au nanoparticles are uniformly anchored on carbon nanotubes to afford substantially increased current density, improved selectivity for CO, and enhanced stability...
February 14, 2019: ChemSusChem
Zongzhao Sun, Yabin Jiang, Lei Zeng, Limin Huang
Inspired by D-A polymers in organic solar cell and extended conjugate effect, a conceptual design of D-π-A type mesoporous carbon nitride with benzene or thiophene as π-spacer is proposed as an efficient photocatalyst for hydrogen evolution and successfully synthesized in one-pot thermopolymerization based on nucleophilic substitution and Schiff base chemical reaction. On the molecular level, the inserted in-plane benzene as π-spacer by forming covalent bonds C=N (acceptor) and C-N (donor) interrupts the continuity of 3, s-triazine units while it maintains the intrinsic π-π conjugated electronic system...
February 13, 2019: ChemSusChem
Anna Lenarda, Manuela Bevilacqua, Claudio Tavagnacco, Lucia Nasi, Alejandro Criado, Francesco Vizza, Michele Melchionna, Maurizio Prato, Paolo Fornasiero
Electrocatalytic oxygen reduction (ORR) is an emerging synthetic strategy to prepare hydrogen peroxide (H2O2) in a sustainable fashion. N-doped graphitic carbon embedding cobalt nanoparticles is selected as an advanced material able to selectively trigger the ORR to form H2O2 with a Faraday Efficiency of almost 100% at very positive applied potentials. The production of H2O2 proceeds with high rates as calculated by bulk electrolysis (49 mmol g-1 h-1) and excellent current densities (about -0.8 mA cm-2 at 0...
February 13, 2019: ChemSusChem
Andrey Shatskiy, Andrey Bardin, Michael Oschmann, Roc Matheu, Jordi Benet-Bucholz, Lars Eriksson, Markus Kärkäs, Eric Johnston, Carolina Gimbert-Suriñach, Antoni Llobet, Björn Åkermark
Herein is described a highly active ruthenium-based water oxidation catalyst [RuX(mcbp)(OHn)(py)2] (5, mcbp2- = 2,6-bis(1-methyl-4-(carboxylate)benzimidazol-2-yl)pyridine; n = 2, 1, and 0 for X = II, III, and IV, respectively), which can be generated in a mixture of RuIII/RuIV states from either [RuII(mcbp)(py)2] (4II) or [RuIII(Hmcbp)(py)2]2+ (4III). Complexes 4II and 4III were isolated and characterized by single crystal X-ray analysis, NMR, UV-vis, FT-IR, ESI-HRMS, EPR, and elemental analysis, and their redox properties were studied in detail by electrochemical and spectroscopic methods...
February 13, 2019: ChemSusChem
Charl J Jafta, Bishnu P Thapaliya, Hailong Lyu, Jiexiang Xia, Harry M Meyer, Mariapan Parans Paranthaman, Xiao-Guang Sun, Craig A Bridges, Sheng Dai
Herein we show, for the first time, the transformation of MXene sheets into TiOF2 2D sheets with superior electrochemical performance. MXene synthesized from Ti3AlC2 has been fluorinated for 3-, 6-, and 24 hours, respectively, by means of a direct fluorination process. Exposure of MXene powder to elemental fluorine for 3 hours induces the formation of CF2 groups and TiF3 on the surface, which have beneficial effects on the electrochemical performance. X-ray photoelectron spectroscopy suggests that after fluorinating the MXene sample for 6 hours, that 2+ and 3+ Ti oxidation states are not present on the surface, with only Ti4+ present indicating TiOF2...
February 13, 2019: ChemSusChem
Bingqing Zhang, Lihue He, Tingting Yao, Wenjun Fan, Xiangtian Zhang, Sheng Wen, Jingying Shi, Can Li
The photoelectrochemical (PEC) method offers an alternative approach to photovoltaic devices for solar electricity generation. The water oxidation reaction (WOR) on the anode and oxygen reduction reaction (ORR) on the cathode is an ideal design for energy transfer owing to their superiority in terms of cleanliness, eco-friendliness, and natural abundance. However, solar electricity production based on O2 circulation by a fuel-free PEC cell is very challenging because it is extremely hard to extract electrons from water molecules owing to the uphill and sluggish WOR together with enormous overpotential for the cathodic ORR...
February 12, 2019: ChemSusChem
Yunjian Ma, Peilin Li, Sébastien J-P Willot, Wuyuan Zhang, Doris Ribitsch, Young Hae Choi, Tianyu Zhang, Robert Verpoort, Frank Hollmann, Yonghua Wang
We report the use of Natural Deep Eutectic Solvents (NADES) as multifunctional solvents for limonene bioprocessing: for the extraction of limonene from orange peel wastes, as solvent for the chemoenzymatic epoxidation of the limonene and as sacrificial electron donor for the in situ generation of H2O2 to promote the epoxidation reaction. The proof of concept for this multifunctional use is provided and the scope and current limitations of the concept are outlined.
February 11, 2019: ChemSusChem
Di-Chang Zhong, Dong-Cheng Liu, Ting Ouyang, Ran Xiao, Wen-Ju Liu, Zhengtao Xu, Tong-Bu Lu
Using solar energy to convert CO2 into valuable fuels or chemicals offers a powerful solution to the urgent energy and environment problems. However, the development of efficient and selective catalysts remains a considerable scientific challenge. Herein, we report a versatile strategy for anchoring catalytically active Co(II) centers into the porous matrix of metal-organic frameworks (MOFs), by utilizing a robust Zr-based MOF (Zr-DMBD) functionalized with self-standing thiol (-SH) groups to enable efficient post-synthetic metal insertion...
February 11, 2019: ChemSusChem
Shammi Akter Ferdousi, Matthias Hilder, Andrew Basile, Haijin Zhu, Luke A O'Dell, Damien Saurel, Teofilo Rojo, Michel Armand, Maria Forsyth, Patrick Howlett
The effect of water on the properties of super concentrated sodium salt solutions in ionic liquids (ILs) was investigated in order to design electrolytes for sodium battery applications using water as an additive. Water were added to a 50 mol% solution of NaFSI in the ionic liquid N-methyl-N-propylpyrrolidinium bis(fluorosulfonyl)imide (C3mpyrFSI). While the thermal properties (glass transition temperature) showed little dependence on the water content, the viscosity and, in particular the ionic conductivity, are strongly affected...
February 10, 2019: ChemSusChem
Gonzalo de Gonzalo, Andrés R Alcántara, Pablo Domínguez de María
The quest of sustainable solvents is currently matter of intense research and development, as solvents significantly contribute to the wastes generated by chemical industries. Cyclopentyl-methyl ether (CPME) is a promising eco-friendly solvent, because of its valuable properties such as low peroxide formation rate, stability at basic and acidic conditions, relatively high boiling point, etc. This review discusses the potential use of CPME for applications in Biotechnology (e.g. biotransformations, as solvent or co-solvent), Biorefineries and Bioeconomy (e...
February 8, 2019: ChemSusChem
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