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Julia Schuster, Jonas Muessig, Rian D Dewhurst, Holger Braunschweig
A range of double carbene adducts of digallanes(4) are prepared from an existing double digallane adduct, and their halides are subsequently exchanged, establishing the feasibility of both base and halide exchange reactions from digallane adducts. Furthermore, a range of digallium species are treated with transition metal Lewis bases, leading alternatively to oxidative addition products, species with monocoordinate Ga+ ligands, and an unusual ditopic metal-only Lewis pair (MOLP). These results underline the manifold and unpredictable chemistry of halogallane species with Lewis bases...
April 18, 2018: Chemistry: a European Journal
Valerie Seymour, Stephen Day, Gudrun Scholz, Kerstin Scheurell, Dinu Iuga, John Griffin, Erhard Kemnitz, John Hanna, Mark E Smith
Multinuclear (1H, 13C, 25Mg) solid-state NMR data is reported for a series of magnesium acetate phases Mg(CH3COO)2.nH2O (n = 0 (two polymorphs), 1, 4). The central focus here is 25Mg as this set of compounds provides an expanded range of local magnesium coordinations compared to what has previously been reported in the literature using NMR. These four compounds provide 10 distinct magnesium sites with varying NMR interaction parameters. One of the anhydrous crystal structures (α) has an MgO7 site which is reported, to the best of our knowledge, for the first time...
April 18, 2018: Chemphyschem: a European Journal of Chemical Physics and Physical Chemistry
Bowen Lei, Xiaojiao Wang, Lifang Ma, Yan Li, Ziyuan Li
An iron-catalysed intermolecular vicinal aminoazidation of alkenes, using N-fluorobenzenesulfonimide (NFSI) and trimethylsilyl azide (TMSN3) as the imidating and azidating reagents, respectively, is described, which could potentially provide a valuable route toward diverse vicinal diamine derivatives of great significance in medicinal chemistry and organic synthesis. Such iron-catalysed aminative bisfunctionalization of alkenes with NFSI has not been reported yet. Comparing to previously employed copper or palladium catalysts, the iron catalyst, FeCl2, was demonstrated to be a good alternative for its comparable efficiency and broad alkene scope...
April 18, 2018: Organic & Biomolecular Chemistry
Xiaoming Zhang, Tianwei Gu, Shaodong Shi, Leyi Li, Shansheng Yu
Pt monolayer catalyst could greatly reduce the use of platinum. However, the core or subsurface transition metal could easily segregate to the surface and eventually selectively dissolve in the working conditions. In this work, a type of PtML /MML /WC multi-layer structure catalyst has been designed using DFT method. The results show that the stability of W-terminated core catalysts is lower than that of the corresponding C-terminated one. More importantly, C-terminated PtML/CoML/WC alloy could also maintain a stable platinum monolayer structure in various electrolyte solutions (eg, perchloric acid, phosphoric acid, alkaline solutions) and via different ORR pathways, in addition to the previously well-known precious alloy elements, such as Ru, Ir, etc...
April 18, 2018: ACS Applied Materials & Interfaces
Xueqing Liu, Sha Peng, Shuyu Gao, Yuancheng Cao, Qingliang You, Liyong Zhou, Yongcheng Jin, Zhihong Liu, Jiyan Liu
It is of great significance to seek high performance solid electrolytes via a facile chemistry and simple process for meeting the requirements of solid batteries. Previous reports revealed that ion conducting pathways within ceramic-polymer composite electrolytes mainly occur at ceramic particles and the ceramic-polymer interface. Herein, one facile strategy towards ceramic particles alignment and assembly induced by an external alternating-current electric-field were presented. It was manifested by in-situ optical microscope that Li1...
April 18, 2018: ACS Applied Materials & Interfaces
Guosheng Liu, Fei Wang, Dinghai Wang, Ling Liang, Ronghua Lu, Pinhong Chen, Zhenyang Lin, Yu Zhou
A ligand-controlled system that enables regioselective trifluoromethylcyanation of 1,3-enynes has been identified, which provides an access to a variety of CF3-containing tri- and tetra-substituted allenyl nitriles. We disclose that the involved propargylic radicals can be selectively trapped by (Box)Cu(II) cyanide, while the tautomerized allenyl radicals are trapped by (phen)Cu(II) cyanide. In addition, the reaction features broad substrate scope and excellent functional group compatibility. Moreover, this protocol represents a novel regioselectivity-tunable functionalization of 1,3-enynes via radicals, which we believe will have great potential implications for the development of catalytic systems for selectivity control in radical and organometallic chemistry...
April 17, 2018: Angewandte Chemie
Cheng Zou, Jingxia Wang, Meng Wang, Yuchen Wu, Kehua Gu, Zhihao Shen, Guirong Xiong, Huai Yang, Lei Jiang, Tomiki Ikeda
The large-area formation of functional micropatterns with liquid crystals is of great significance for diversified applications in interdisciplinary fields. Meanwhile, the control of molecular alignment in the patterns is fundamental and prerequisite for the adequate exploitation of their photoelectric properties. However, it would be extremely complicated and challenging for discotic liquid crystals (DLCs) to achieve the goal, because they are insensitive to external fields and surface chemistry. Herein, a simple method of patterning and aligning DLCs on flat substrates is disclosed through precise control of the formation and dewetting of the capillary liquid bridges, within which the DLC molecules are confined...
April 18, 2018: Small
A A Tabolin, A Yu Sukhorukov, S L Ioffe
Chemistry of covalent nitronates regarding nucleophilic addition to C=N bond is described. Various types of electrophilic activation of nitronates and stability of formed products are discussed with main attention paid to authors' work in the area.
April 18, 2018: Chemical Record: An Official Publication of the Chemical Society of Japan ... [et Al.]
Xingang Zhang, Lun An, Yu-Lan Xiao, Shu Zhang
Although iron-catalyzed cross-coupling of Grignard reagents with alkyl halides has been well established, the adoption of the reaction for fluoroalkylations has not been reported because traditional catalytic systems often lead to defluorination reactions. Here, we describe our investigation of an iron-catalyzed cross-coupling between arylmagnesium and difluoroalkyl bromides with steric modified N,N,N',N'-tetramethyl-ethane-1,2-diamine (TMEDA) (L4) as a ligand. The use of a bulky diamine ligand (L4), in which a butylene is substituted at one carbon atom of ethylene backbone in TMEDA, enables the iron-catalyzed difluoroalkylation under mild reaction conditions with a wide range of difluoroalkyl bromides including vulnerable bromodifluoromethane, thus providing a general and cost-efficient route for application in medicinal chemistry...
April 17, 2018: Angewandte Chemie
Jing-Xuan Zhang, Fu Kit Sheong, Zhenyang Lin
Decomposing chemical interactions into bonds and other higher order interactions is a common practice to analyse chemical structures and gave birth to many chemical concepts despite the fact that the decomposition itself might be subjective in nature. Fragment molecular orbitals (FMOs) offer a more rigorous alternative to such intuition, but might be less interpretable due to extensive delocalisation in FMOs. Inspired by the Principal Component Analysis in statistics, we hereby present a novel framework, Principal Interacting Orbital (PIO) analysis, that can very quickly identify the "dominant interacting orbitals" that are semi-localised and easily interpretable while still maintaining the mathematical rigor...
April 17, 2018: Chemistry: a European Journal
Yupeng He, Shifeng Hou, Liqiong Yang, Fang Zhang, Guizheng Zou
Tunable optics and electronics of II-VI nanocrystals (NCs) is mainly achieved in the traditional size-dependent strategy. Herein, adjustable triggering energy, intensity, and even spectrum for reductive-oxidation electrochemiluminescence (ECL) from highly-passivated CdTe/CdS NCs of the same size are achieved via decorating NCs with counterions, which proves surface chemistry can bring out varied electrostatic interaction between surface vacancies and electrochemically injected carriers for adjustable electrochemical redox induced radiative charge-transfer...
April 17, 2018: Chemistry: a European Journal
Tsiverihasina V Rakotonimaro, Carmen Mihaela Neculita, Bruno Bussière, Thomas Genty, Gérald J Zagury
Multi-step passive systems for the treatment of iron-rich acid mine drainage (Fe-rich AMD) perform satisfactorily at the laboratory scale. However, their field-scale application has revealed dissimilarities in performance, particularly with respect to hydraulic parameters. In this study, the assessment of factors potentially responsible for the variations in performance of laboratory and field-scale multi-step systems was undertaken. Three laboratory multi-step treatment scenarios, involving a combination of dispersed alkaline substrate (DAS) units, anoxic dolomitic drains, and passive biochemical reactors (PBRs), were set up in 10...
April 17, 2018: Environmental Science and Pollution Research International
Lorenzo Angiolini, Sabrina Valetti, Boiko Cohen, Adam Feiler, Abderrazzak Douhal
We report on the encapsulation of the antibiotic clofazimine (CLZ) within the pores of mesoporous silica particles having hydrophilic (CBET value of 137) and more hydrophobic (CBET value of 94 after calcination at 600 °C) surfaces. We studied the effect of pH on the released amount of CLZ in aqueous solutions and observed a maximum at pH 4.1 in correlation with the solubility of the drug. Less release of the drug was observed from the more hydrophobic particles which was attributed to a difference in the affinity of the drug to the carrier particles...
April 18, 2018: Physical Chemistry Chemical Physics: PCCP
Daiheon Lee, Joseph P Park, Mi-Young Koh, Pureum Kim, Junhee Lee, Mikyung Shin, Haeshin Lee
Mussel-inspired adhesive coatings on biomedical devices have attracted significant interest due to their unique properties such as substrate independency and high efficiency. The key molecules for mussel-inspired adhesive coatings are catechol and amine groups. Along with the understanding of catechol chemistry, chitosan-catechol has also been developed as a representative mussel-inpired adhesive polymer that contains catechol and amine groups for adhesiveness. Herein, we demonstrated the direct writability of chitosan-catechol as a bioink for 3D printing, one of the additive techniques...
April 18, 2018: Biomaterials Science
Roland C Fischer, Michael S Hill, David J Liptrot
No abstract text is available yet for this article.
April 18, 2018: Dalton Transactions: An International Journal of Inorganic Chemistry
Terrance J Hadlington, Matthias Driess, Cameron Jones
The chemistry of group 14 element(ii) hydride complexes has rapidly expanded since the first stable example of such a compound was reported in 2000. Since that time it has become apparent that these systems display remarkable reactivity patterns, in some cases mimicking those of late transition-metal (TM) hydride compounds. This is especially so for the hydroelementation of unsaturated organic substrates. Recently, this aspect of their reactivity has been extended to the use of group 14 element(ii) hydrides as efficient, "TM-like" catalysts in organic synthesis...
April 18, 2018: Chemical Society Reviews
Patricia M Valdespino-Castillo, Ping Hu, Martín Merino-Ibarra, Luz M López-Gómez, Daniel Cerqueda-García, Roberto González-De Zayas, Teresa Pi-Puig, Julio A Lestayo, Hoi-Ying Holman, Luisa I Falcón
Microbialites are modern analogs of ancient microbial consortia that date as far back as the Archaean Eon. Microbialites have contributed to the geochemical history of our planet through their diverse metabolic capacities that mediate mineral precipitation. These mineral-forming microbial assemblages accumulate major ions, trace elements and biomass from their ambient aquatic environments; their role in the resulting chemical structure of these lithifications needs clarification. We studied the biogeochemistry and microbial structure of microbialites collected from diverse locations in Mexico and in a previously undescribed microbialite in Cuba...
2018: Frontiers in Microbiology
Anne Marie Dupuy, Stéphanie Badiou, Delphine Daubin, Anne Sophie Bargnoux, Chloé Magnan, Kadda Klouche, Jean Paul Cristol
Introduction: Obtaining suitable results unaffected by pre- or postanalytical phases is pivotal for clinical chemistry service. We aimed comparison and stability of nine biochemical analytes after centrifugation using Barricor™ plasma tubes with mechanical separator vs standard Vacutainer® lithium heparin tubes. Materials and methods: We collected samples on six healthy volunteers and nine patients from intensive care units into 6 mL plastic Vacutainer® lithium heparin tubes and 5...
June 15, 2018: Biochemia Medica: časopis Hrvatskoga Društva Medicinskih Biokemičara
Nadine Sobotzki, Michael A Schafroth, Alina Rudnicka, Anika Koetemann, Florian Marty, Sandra Goetze, Yohei Yamauchi, Erick M Carreira, Bernd Wollscheid
Cellular responses depend on the interactions of extracellular ligands, such as nutrients, growth factors, or drugs, with specific cell-surface receptors. The sensitivity of these interactions to non-physiological conditions, however, makes them challenging to study using in vitro assays. Here we present HATRIC-based ligand receptor capture (HATRIC-LRC), a chemoproteomic technology that successfully identifies target receptors for orphan ligands on living cells ranging from small molecules to intact viruses...
April 17, 2018: Nature Communications
Ganna Gryn'ova, Clémence Corminboeuf
Molecular electronics covers several distinctly different conducting architectures, including organic semiconductors and single-molecule junctions. The non-covalent interactions, abundant in the former, are also often found in the latter, i.e. the dimer junctions. In the present work, we draw the parallel between the two types of non-covalent molecular electronics for a range of π-conjugated heteroaromatic molecules. In silico modeling allows us to distill the factors that arise from the chemical nature of their building blocks and from their mutual arrangement...
April 17, 2018: Journal of Physical Chemistry Letters
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