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911.
Mechanistic Insights into the Post‐Cyclization Isomerization in Gold‐Catalyzed 7‐exo‐dig‐Hydroarylations
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M. Sc. Daniel Pflästerer Sören Schumacher Dr. Matthias Rudolph Prof. Dr. A. Stephen K. Hashmi 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(32):11585-11589
The subsequent double‐bond isomerization in the synthesis of dibenzocycloheptenes and their heteroaromatic analogues was investigated. In the case of biphenyls, a basic additive completely prevented an isomerization to the thermodynamic product. With electron‐rich intramolecular heteroaromatic nucleophiles, the isomerization was still observed, but the kinetic product can be obtained by careful control of the reaction times in most cases. Mechanistic studies demonstrated that a slow isomerization is also possible with the gold catalyst at elevated temperatures, but much faster isomerization rates were observed with acidic additives. An observed initiation period for the gold‐catalyzed isomerization indicates that not the homogenous catalyst, but a decomposition product of it may be the catalytically active species. 相似文献
912.
Enhanced Photocatalytic Reduction of CO2 to CO through TiO2 Passivation of InP in Ionic Liquids
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Guangtong Zeng Jing Qiu Bingya Hou Haotian Shi Dr. Yongjing Lin Mark Hettick Prof. Ali Javey Prof. Stephen B. Cronin 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(39):13502-13507
A robust and reliable method for improving the photocatalytic performance of InP, which is one of the best known materials for solar photoconversion (i.e., solar cells). In this article, we report substantial improvements (up to 18×) in the photocatalytic yields for CO2 reduction to CO through the surface passivation of InP with TiO2 deposited by atomic layer deposition (ALD). Here, the main mechanisms of enhancement are the introduction of catalytically active sites and the formation of a pn‐junction. Photoelectrochemical reactions were carried out in a nonaqueous solution consisting of ionic liquid, 1‐ethyl‐3‐methylimidazolium tetrafluoroborate ([EMIM]BF4), dissolved in acetonitrile, which enables CO2 reduction with a Faradaic efficiency of 99 % at an underpotential of +0.78 V. While the photocatalytic yield increases with the addition of the TiO2 layer, a corresponding drop in the photoluminescence intensity indicates the presence of catalytically active sites, which cause an increase in the electron‐hole pair recombination rate. NMR spectra show that the [EMIM]+ ions in solution form an intermediate complex with CO2?, thus lowering the energy barrier of this reaction. 相似文献
913.
Total Synthesis of cis‐Clavicipitic Acid from Asparagine via Ir‐Catalyzed CH bond Activation as a Key Step
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Yu‐ki Tahara Mamoru Ito Dr. Kyalo Stephen Kanyiva Prof. Dr. Takanori Shibata 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(32):11340-11343
4‐Substituted tryptophan derivatives and the total synthesis of cis‐clavicipitic acid were achieved in reactions in which Ir‐catalyzed C?H bond activation was a key step. The starting material for these reactions is asparagine, which is a cheap natural amino acid. The reductive amination step from the 4‐substituted tryptophan derivative gave cis‐clavicipitic acid with perfect diastereoselectivity. 相似文献
914.
Dr. Igor V. Pimkov Dr. Barbara Serli‐Mitasev Antoinette A. Peterson Stephen C. Ratvasky Dr. Bernd Hammann Prof. Partha Basu 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(47):17057-17072
Molybdopterin is an essential cofactor for all forms of life. The cofactor is composed of a pterin moiety appended to a dithiolene‐functionalized pyran ring, and through the dithiolene moiety it binds metal ions. Different synthetic strategies for dithiolene‐functionalized pyran precursors that have been designed and synthesized are discussed. These precursors also harbor 1,2‐diketone or osone functionality that has been condensed with 1,2‐diaminobenzene or other heterocycles resulting in several quinoxaline or pterin derivatives. Use of additives improves the regioselectivity of the complexes. The molecules have been characterized by 1H and 13C NMR and IR spectroscopies, as well as by mass spectrometry. In addition, several compounds have been crystallographically characterized. The geometries of the synthesized molecules are more planar than the geometry of the cofactor found in proteins. 相似文献
915.
916.
Adrian Boborodea Stephen O’Donohue 《International Journal of Polymer Analysis and Characterization》2017,22(7):631-638
A new evaporative light scattering detector (ELSD) for the analysis of polyolefins by high temperature gel permeation chromatography (GPC) was recently introduced by Agilent Technologies. For the first time, we investigated the possibility to use this detector to measure the molecular weight distributions (MWD) of different type of polyolefines (polypropylene, linear, and low-density polyethylene). These samples were previously characterized by GPC with a differential refractive index (DRI) detector by several companies, in an interlaboratory study conducted by International Union of Pure and Applied Chemistry.[1] The excellent baseline stability of ELSD as compared with DRI was reflected in a better reproducibility of the measured average molecular weights. More importantly, after applying required corrections to linearize the response of the ELSD as a function of concentration, we obtained similar results as previously obtained with DRI for the MWD of analyzed resins, covering typical applications of polyolefins. 相似文献
917.
Barwick Vicki Ellison Stephen L. R. Gjengedal Elin Magnusson Bertil Molinier Olivier Patriarca Marina Sibbesen Lorens Vanlaethem Nicole Vercruysse Isabelle 《Accreditation and quality assurance》2017,22(5):253-263
Accreditation and Quality Assurance - Eurachem held a workshop on method validation in analytical sciences in Gent, Belgium, on 9–10 May 2016. A summary of the working group discussions is... 相似文献
918.
Let X_1 and X_2 be two compact connected strongly pseudoconvex embeddable Cauchy-Riemann(CR) manifolds of dimensions 2m-1 and 2n-1 in C~(m+1)and C~(n+1), respectively. We introduce the ThomSebastiani sum X = X_1 ⊕X_2which is a new compact connected strongly pseudoconvex embeddable CR manifold of dimension 2m+2n+1 in C~(m+n+2). Thus the set of all codimension 3 strongly pseudoconvex compact connected CR manifolds in Cn+1for all n 2 forms a semigroup. X is said to be an irreducible element in this semigroup if X cannot be written in the form X_1 ⊕ X_2. It is a natural question to determine when X is an irreducible CR manifold. We use Kohn-Rossi cohomology groups to give a necessary condition of the above question. Explicitly,we show that if X = X_1 ⊕ X_2, then the Kohn-Rossi cohomology of the X is the product of those Kohn-Rossi cohomology coming from X_1 and X_2 provided that X_2 admits a transversal holomorphic S~1-action. 相似文献
919.
Journal of Solid State Electrochemistry - 相似文献
920.
Stephen L. Jones 《International Journal of Mathematical Education in Science & Technology》2017,48(2):300-306
Dr RL Moore was undoubtedly one of the finest mathematics teachers ever. He developed a unique teaching method designed to teach his students to think like mathematicians. His method was not designed to convey any particular mathematical knowledge. Instead, it was designed to teach his students to think. Today, his method has been modified to focus on using student participation toward the goal of the conveyance of mathematical knowledge rather than on Dr Moore's goal of teaching students to think. This article proposes that undergraduates would be better served if they took at least one course using Dr Moore's original method and his original goal. 相似文献