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https://www.readbyqxmd.com/read/28741940/directed-%C3%AE-c-h-amination-of-alcohols-via-radical-relay-chaperones
#1
Ethan A Wappes, Kohki M Nakafuku, David A Nagib
A radical-mediated strategy for β C-H amination of alcohols has been developed. This approach employs a radical relay chaperone, which serves as a traceless director that facilitates selective C-H functionalization via 1,5-hydrogen atom transfer (HAT) and enables net incorporation of ammonia at the β carbon of alcohols. The chaperones presented herein enable direct access to imidate radicals, allowing their first use for H atom abstraction. A streamlined protocol enables rapid conversion of alcohols to their β-amino analogs (via in situ conversion of alcohols to imidates, directed C-H amination, and hydrolysis to NH2)...
July 25, 2017: Journal of the American Chemical Society
https://www.readbyqxmd.com/read/28739436/efficacy-of-isoniazid-salvage-therapy-for-latent-tuberculosis-infection-in-patients-with-immune-mediated-inflammatory-disorders-a-retrospective-cohort-study-in-taiwan
#2
Shiang-Fen Huang, Ming-Han Chen, Fu-Der Wang, Chang-Youh Tsai, Chang-Phone Fung, Wei-Juin Su
BACKGROUND: Active tuberculosis (TB) in patients with latent tuberculosis infection (LTBI) was associated with use of biological agents for immune-mediated inflammatory disorders (IMIDs). For decreasing active TB, isoniazid prophylaxis therapy was administered before biologic therapy among IMID patients with LTBI. However, for patients who had been received biologics for a long time with unknown status of LTBI or exposure history of active TB, the prevalence of LTBI and efficacy of isoniazid therapy were unclear...
June 29, 2017: Journal of Microbiology, Immunology, and Infection, Wei Mian Yu Gan Ran za Zhi
https://www.readbyqxmd.com/read/28734209/new-insight-into-the-environmental-impact-of-two-imidazolium-ionic-liquids-effects-on-seed-germination-and-soil-microbial-activity
#3
J Salgado, J J Parajó, T Teijeira, O Cruz, J Proupín, M Villanueva, J A Rodríguez-Añón, P V Verdes, O Reyes
The next generation of ionic liquids must be synthetized taking into account structures that guarantee the suitable properties for a defined application as well as ecological data. Thus, searching of the right methodologies to know, quickly and efficiently, the ecological effects of these compounds is a preliminary task. The effects of two imidazolium based ionic liquids with different anions, 1-butyl-3-methylimidazolium tetrafluoroborate, [C4C1Im][BF4], and 1-propyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide, [C3C1Im][NTf2], on seedling emergence of six tree species and on the microbial behaviour of two soils were determined in this work...
July 14, 2017: Chemosphere
https://www.readbyqxmd.com/read/28731317/air-stable-self-bleaching-electrochromic-device-based-on-viologen-and-ferrocene-containing-triflimide-redox-ionic-liquids
#4
Bruno Gélinas, Dyuman Das, Dominic Rochefort
We demonstrate an electrochromic device with self-bleaching ability that uses ethyl viologen- ([EV](2+)) and ferrocene-based redox ionic liquids ([FcNTf](-)) as the electroactive species. These electroactive compounds are insensitive to atmospheric O2 and H2O in both their oxidized and reduced states once dissolved in a typical ionic liquid electrolyte ([BMIm][NTf2]), allowing for the device to be assembled outside a glovebox without any encapsulation. This device could generate a deep blue color by applying a 2...
July 21, 2017: ACS Applied Materials & Interfaces
https://www.readbyqxmd.com/read/28726865/recent-advances-in-the-ruthenium-ii-catalyzed-chelation-assisted-c-h-olefination-of-substituted-aromatics-alkenes-and-heteroaromatics-with-alkenes-via-the-deprotonation-pathway
#5
Rajendran Manikandan, Masilamani Jeganmohan
The transition-metal-catalyzed chelation-assisted alkenylation at the inert C-H bond of aromatics with alkenes is one of the efficient methods to synthesize substituted vinylarenes in a highly regio- and stereoselective manner. Palladium, rhodium and ruthenium complexes are frequently used as catalysts for this type of transformation. The present review describes the recent advances in the ruthenium-catalyzed chelation-assisted alkenylation at the C-H bond of aromatics, alkenes and heteroaromatics with alkenes via the deprotonation pathway...
July 20, 2017: Chemical Communications: Chem Comm
https://www.readbyqxmd.com/read/28723222/extraction-of-2-phenylethanol-pea-from-aqueous-solution-using-ionic-liquids-synthesis-phase-equilibrium-investigation-selectivity-in-separation-and-thermodynamic-models
#6
Urszula Maria Domanska, Patrycja Okuniewska, Kamil Paduszyński, Marta Królikowska, Maciej Zawadzki, Mikolaj Wieckowski
This work presents some important issues and topics related to possible extraction of 2-phenylethanol (PEA) from aqueous phase "in situ" during the biosynthesis. It consist of a series of experimental phase equilibrium measurements in binary and ternary systems. Ionic liquids (ILs) are an important new media for imaging and sensing applications because of their solvation property, thermal stability and negligible vapor pressure. However, complex procedures and non-miscibility with water are often required in PEA extraction...
July 19, 2017: Journal of Physical Chemistry. B
https://www.readbyqxmd.com/read/28723129/carbon-dioxide-in-a-supported-ionic-liquid-membrane-structural-and-rotational-dynamics-measured-with-2d-ir-and-pump-probe-experiments
#7
Jae Yoon Shin, Steven A Yamada, Michael D Fayer
Supported ionic liquid membranes (SILMs) are porous membranes impregnated with ionic liquids (ILs) and used as advanced carbon capture materials. Here, two-dimensional infrared (2D IR) and IR polarization selective pump-probe (PSPP) spectroscopies were used to investigate CO2 reorientation and spectral diffusion dynamics in SILMs. The SILM contained 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonly)imide in the poly(ether sulfone) membrane with average pore size of ~350 nm. Two ensembles of CO2 were observed in the SILM, one in the IL phase in the membrane pores and the other in the supporting membrane polymer...
July 19, 2017: Journal of the American Chemical Society
https://www.readbyqxmd.com/read/28718978/effective-charges-of-ionic-liquid-determined-self-consistently-through-combination-of-molecular-dynamics-simulation-and-density-functional-theory
#8
Ryosuke Ishizuka, Nobuyuki Matubayasi
A self-consistent scheme combining the molecular dynamics (MD) simulation and density functional theory (DFT) was recently proposed to incorporate the effects of the charge transfer and polarization of ions into non-poralizable force fields of ionic liquids for improved description of energetics and dynamics. The purpose of the present work is to analyze the detailed setups of the MD/DFT scheme by focusing on how the basis set, exchange-correlation (XC) functional, charge-fitting method or force field for the intramolecular and Lennard-Jones interactions affects the MD/DFT results of 1,3-dimethylimidazolium bis(trifluoromethylsulfonyl) imide ( [C1mim][NTf2]) and 1-ethyl-3-methylimidazolium glycinate ( [C2mim][Gly])...
July 18, 2017: Journal of Computational Chemistry
https://www.readbyqxmd.com/read/28715188/understanding-microscopic-behavior-of-the-mixture-of-ionic-liquid-ethylene-glycol-lithium-salt-through-time-resolved-fluorescence-nuclear-magnetic-resonance-nmr-and-electron-paramagnetic-resonance-epr-studies
#9
Ranu Satish Dhale, Prabhat Kumar Sahu, Moloy Sarkar
The present study has been undertaken with an aim to find out the suitability of a binary solvent system, comprising an ionic liquid, 1-(2-Hydroxyethyl)-3-methylimidazolium bis (trifluoromethylsulfonyl)imide ([OHEMIM][NTf2]) and ethylene glycol (EG), towards lithium ion battery applications. For this purpose, the behavior in terms of structure, intermolecular interaction and dynamics of several solvent systems, [OHEMIM][NTf2], [OHEMIM][NTf2]-LiNTf2(lithium bis(trifluoromethylsulfonyl)imide), [OHEMIM][NTf2]-EG and [OHEMIM][NTf2]-EG-LiNTf2 are investigated by carrying out steady state and time-resolved fluorescence, nuclear magnetic resonance (NMR) and electron paramagnetic resonance (EPR) measurements...
July 17, 2017: Journal of Physical Chemistry. B
https://www.readbyqxmd.com/read/28714310/rapid-high-yielding-syntheses-of-crown-ether-based-pyridyl-cryptands
#10
Terry Leon Price, Hanlie Ronel Wessels, Carla Slebodnick, Harry William Gibson
Pyridinium bis(trifluoromethylsulfonyl)imide (PyTFSI) templated syntheses of 2,6-pyridyl cryptands of cis(4,4')-dibenzo-30-crown-10 (3a), the p-bromobenzyloxy derivative 3b, bis(m-phenylene)-32-crown-10 (5), cis(4,4')-dibenzo-27S-crown-9 (7), cis(4,4')-dibenzo-27L-crown-9 (9) and cis(4,4')-dibenzo-24-crown-8 (11) are reported. Here we provide a fast (12 h), high yielding (89, 74, 80 and 62 % for 3a, 3b, 5 and 9, respectively) templation method without the use of a syringe pump. The yields for 7 (19 %) and 11 (26 %) were lower than with the previous pseudo-high dilution method, indicating ineffective templation in these cases...
July 17, 2017: Journal of Organic Chemistry
https://www.readbyqxmd.com/read/28707746/gas-evolution-in-activated-carbon-based-supercapacitors-using-protic-deep-eutectic-solvent-as-electrolyte
#11
Satyajit Phadke, Samia Amara, Meriem Anouti
One of the primary causes of ageing in supercapacitors are the irreversible faradaic reactions occurring near the operating voltage limit which lead to the production of gases resulting in device swelling, increased resistance (ESR), and lowering of the capacitance. In this study, we report a investigation of a protic "Deep Eutectic Solvent" (DES) consisting on mixture of Lithium bis(fluorosulfonyl)imide salt (LiFSI) with formamide (FMD) as H-bond donor (xLiFSI = 0.25 ; C = 2.5 M LiFSI) as electrolyte for AC based EDLC...
July 14, 2017: Chemphyschem: a European Journal of Chemical Physics and Physical Chemistry
https://www.readbyqxmd.com/read/28707619/evaluation-of-gas-chromatography-stationary-phases-based-on-morpholinium-ionic-liquids-by-mcreynolds-constants-and-activity-coefficients-at-infinite-dilution
#12
Kateryna Yavir, Łukasz Marcinkowski, Adam Kloskowski, Jacek Namieśnik
In this work, four ionic liquids (ILs) based on the N-alkyl-N-methylmorpholinium cation ([Mor1,R], in which R = 2, 4, 8, or 10) and bis(trifluoromethanesulfonyl)imide anion were synthesized. Using GLC, a number of parameters describing the sorption properties of the investigated ILs were determined. The values of Kovats indices, McReynolds constants, and activity coefficients at infinite dilution were the basis for the evaluation of intermolecular interactions. The effect of the chain length of the alkyl substituent in the cation, which was used to modify their polarity, has been discussed...
July 13, 2017: Journal of AOAC International
https://www.readbyqxmd.com/read/28704995/molecular-dynamics-simulations-of-amide-functionalized-imidazolium-bis-trifluoromethanesulfonyl-imide-dicationic-ionic-liquids
#13
Hassan Khakan, Saeid Yeganegi
In the present study the structure and dynamics of three dicationic ionic liquids (DILs) with a functional amide group in the imidazolium ring with bis(trifluoromethanesulfonyl)imide, [TFSI]- anion has been studied by molecular dynamics simulations. Densities, radius distribution functions (RDFs), combined distribution functions (CDFs), spatial distribution functions (SDFs), mean-square displacements (MSD), and self-diffusivities for the ions have been calculated from MD simulations. The calculated densities for [C4(amim)2][TFSI]2 at different temperatures agreed well with the experimental values...
July 14, 2017: Journal of Physical Chemistry. B
https://www.readbyqxmd.com/read/28704044/new-scandium-borylimido-chemistry-synthesis-bonding-and-reactivity
#14
Benjamin A Clough, Simona Mellino, Eric Clot, Philip Mountford
We report a combined synthetic, mechanistic and theoretical study of the first borylimido complex of a rare earth metal, (NacNacNMe2)Sc{NB(NAr'CH)2} (25, Ar' = 2,6-C6H3iPr2, NacNacNMe2 = Ar'NC(Me)CHC(Me)NCH2CH2NMe2). Thermolysis of the methyl-borylamide (NacNacNMe2)Sc(Me){NHB(NAr'CH)2} (18) generated transient imide 25 via rate-determining, 1st order methane elimination (KIE ca. 8.7). In the absence of external substrate, 25 underwent a reversible cyclometallation reaction (sp3 C-H bond addition to Sc=Nimide) with a methyl group of the NacNacNMe2 ligand forming {MeC(NC6H3iPrCH(Me)CH2)CHC(Me)NCH2CH2NMe2}-Sc{NHB(NAr'CH)2} (21)...
July 13, 2017: Journal of the American Chemical Society
https://www.readbyqxmd.com/read/28704042/semicrystalline-polymer-binary-phase-structure-templated-quasi-block-graft-copolymers
#15
Jipeng Guan, Yanyuan Wang, Chenyang Xing, Lijun Ye, Yongjin Li, Jingye Li
Herein, we report a simple strategy to synthesize quasi-block graft copolymers using the binary phase structure of semicrystalline polymers as the template. An unsaturated ionic liquid, 1-vinyl-3-butylimidazolium bis (trifluoromethylsulfonyl) imide ([VBIm] [TFSI]), is thermodynamically miscible with poly (vinylidene fluoride-co-hexafluoropropylene) (P(VDF-co-HFP)) in solution. The solidification of P(VDF-co-HFP)/[VBIm] [TFSI] blend leads to the expelling of ILs from the crystalline region and the ILs are only located in the amorphous region...
July 13, 2017: Journal of Physical Chemistry. B
https://www.readbyqxmd.com/read/28703580/complex-permittivity-of-ionic-liquid-mixtures-investigated-by-terahertz-time-domain-spectroscopy
#16
Sen Mou, Andrea Rubano, Domenico Paparo
Ionic liquids are salts found in their liquid state at ambient temperature. The physicochemical properties of ionic liquids can be tailored by selecting constituent cation and anion from numerous available ions. The physicochemical properties can be further tuned by mixing different neat ionic liquids. Reported data of ionic liquid mixtures reveal that frequently investigated properties such as density, viscosity and thermal stability follow corresponding mixing laws. Complex permittivity in the interval of terahertz frequencies is of great importance to understand the molecular interactions and the solvation dynamics which drive the macroscopic properties of ionic liquids, however, to the best of our knowledge, there are scarce reports about the mixing behavior of complex permittivity in ionic liquid mixtures...
July 13, 2017: Journal of Physical Chemistry. B
https://www.readbyqxmd.com/read/28702641/-fefe-hydrogenase-h-cluster-mimics-mediated-by-naphthalene-monoimide-derivatives-of-peri-substituted-dichalcogenides
#17
Hassan Abul-Futouh, Yulian Zagranyarski, Carolin Müller, Martin Schulz, Stephan Kupfer, Helmar Görls, Mohammad El-Khateeb, Stefanie Gräfe, Benjamin Dietzek, Kalina Peneva, Wolfgang Weigand
Synthetic models of the active site of [FeFe]-hydrogenase containing naphthalene monoimide (NMI) of peri-substituted dichalcogenides as bridging linkers have been prepared and characterized using different spectroscopic methods. The influence of the imide functionality and the chalcogen atoms on the redox properties and the catalytic behaviour of complexes 7-10 was studied using cyclic voltammetry. The results revealed that the imide functionality has improved the chemical stability of the reduced species and the replacement of the S atoms by Se caused a cathodic shift in the oxidation peaks...
July 12, 2017: Dalton Transactions: An International Journal of Inorganic Chemistry
https://www.readbyqxmd.com/read/28702548/counterintuitive-trends-of-the-wetting-behavior-of-ionic-liquid-based-electrolytes-on-modified-lithium-electrodes
#18
Paulo Schmitz, Martin Kolek, Diddo Diddens, Marian Cristian Stan, Kirsi Jalkanen, Martin Winter, Peter Bieker
The demand for high energy densities has brought rechargeable lithium metal batteries back into the research focus. Ionic liquids (ILs) are considered as suitable electrolyte components for these systems. In this work, the wetting behavior of 1-ethyl-3-methylimidazolium bis((trifluoromethyl)sulfonyl)imide ([C2MIm]TFSI), 1-butyl-3-methylimidazolium bis-((trifluoromethyl)sulfonyl)imide ([C4MIm]TFSI), 1-hexyl-3-methylimidazolium bis((trifluoromethyl)sulfonyl)imide ([C6MIm]TFSI), and N-butyl-N-methylpyrrolidinium bis((trifluoromethyl)sulfonyl)imide (Pyr14TFSI) on mechanically modified lithium electrodes, with and without lithium bis((trifluoromethyl)sulfonyl)imide (LiTFSI) conducting salt, is investigated and is compared to an organic carbonate-based electrolyte...
July 12, 2017: Physical Chemistry Chemical Physics: PCCP
https://www.readbyqxmd.com/read/28696704/polymer-rich-composite-electrolytes-for-all-solid-state-li-s-cells
#19
Xabier Judez, Heng Zhang, Chunmei Li, Gebrekidan Gebresilassie Eshetu, Yan Zhang, José Antonio González-Marcos, Michel Armand, Lide Mercedez Rodriguez-Martinez
Polymer-rich composite electrolytes with lithium bis(fluorosulfonyl)imide/poly(ethylene oxide) (LiFSI/PEO) containing either Li-ion conducting glass ceramic (LICGC) or inorganic Al2O3 fillers are investigated in all solid-state Li-S cells. In the presence of the fillers, the ionic conductivity of the composite polymer electrolytes (CPEs) does not increase compared to the plain LiFSI/PEO electrolyte at various tested temperatures. The CPE with Al2O3 fillers improves the stability of Li/electrolyte interphase, while the Li-S cell with LICGC-based CPE delivers high sulfur utilization of 1111 mAh g-1 and areal capacity of 1...
July 11, 2017: Journal of Physical Chemistry Letters
https://www.readbyqxmd.com/read/28693317/osmotic-heat-engine-using-thermally-responsive-ionic-liquids
#20
Yujiang Zhong, Xinbo Wang, Xiaoshuang Feng, Selvedin Telalovic, Yves Gnanou, Kuo-Wei Huang, Xiao Hu, Zhiping Lai
The osmotic heat engine (OHE) is a promising technology for converting low grade heat to electricity. Most of the existing studies have focused on thermolytic salt systems. Herein, for the first time, we proposed to use thermally responsive ionic liquids (TRIL) that have either an upper critical solution temperature (UCST) or lower critical solution temperature (LCST) type of phase behavior as novel thermolytic osmotic agents. Closed-loop TRIL-OHEs were designed based on these unique phase behaviors to convert low grade heat to work or electricity...
July 24, 2017: Environmental Science & Technology
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