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11.
Mild Bioconjugation Through the Oxidative Coupling of ortho‐Aminophenols and Anilines with Ferricyanide
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Allie C. Obermeyer John B. Jarman Chawita Netirojjanakul Kareem El Muslemany Prof. Dr. Matthew B. Francis 《Angewandte Chemie (International ed. in English)》2014,53(4):1057-1061
Using a small‐molecule‐based screen, ferricyanide was identified as a mild and efficient oxidant for the coupling of anilines and o‐aminophenols on protein substrates. This reaction is compatible with thiols and 1,2‐diols, allowing its use in the creation of complex bioconjugates for use in biotechnology and materials applications. 相似文献
12.
Igor A. Kaltashov Anton El Khoury Chengfeng Ren Sergey N. Savinov 《Journal of mass spectrometry : JMS》2020,55(2)
Ruthenium is a platinoid that exhibits a range of unique chemical properties in solution, which are exploited in a variety of applications, including luminescent probes, anticancer therapies, and artificial photosynthesis. This paper focuses on a recently demonstrated ability of this metal in its +3 oxidation state to form highly stable complexes with tris (hydroxymethyl)aminomethane (H2NC(CH2OH)3, Tris‐base or T) and imidazole (Im) ligands, where a single RuIII cation is coordinated by two molecules of each T and Im. High‐resolution electrospray ionization mass spectrometry (ESI MS) is used to characterize RuIII complexes formed by placing a RuII complex [(NH3)5RuIICl]Cl in a Tris buffer under aerobic conditions. The most abundant ionic species in ESI MS represent mononuclear complexes containing an oxidized form of the metal, ie, [XnRuIIIT2 – 2H]+, where X could be an additional T (n = 1) or NH3 (n = 0‐2). Di‐ and tri‐metal complexes also give rise to a series of abundant ions, with the highest mass ion representing a metal complex with an empirical formula Ru3C24O21N6H66 (interpreted as cyclo(T2RuO)3, a cyclic oxo‐bridged structure, where the coordination sphere of each metal is completed by two T ligands). The empirical formulae of the binuclear species are consistent with the structures representing acyclic fragments of cyclo(T2RuO)3 with addition of various combinations of ammonia and dioxygen as ligands. Addition of histidine in large molar excess to this solution results in complete disassembly of poly‐nuclear complexes and gives rise to a variety of ionic species in the ESI mass spectrum with a general formula [RuIIIHiskTm (NH3)n ? 2H]+, where k = 0 to 2, m = 0 to 3, and n = 0 to 4. Ammonia adducts are present for all observed combinations of k and m, except k = m = 2, suggesting that [His2RuIIIT2 ? 2H]+ represents a complex with a fully completed coordination sphere. The observed cornucopia of RuIII complexes formed in the presence of histidine is in stark contrast to the previously reported selective reactivity of imidazole, which interacts with the metal by preserving the RuT2 core and giving rise to a single abundant ruthenium complex (represented by [Im2RuIIIT2 ? 2H]+ in ESI mass spectra). Surprisingly, the behavior of a hexa‐histidine peptide (HHHHHH) is similar to that of a single imidazole, rather than a single histidine amino acid: The RuT2 core is preserved, with the following ionic species observed in ESI mass spectra: [HHHHHH·(RuIIIT2)m ? (3m‐1)H]+ (m = 1‐3). The remarkable selectivity of the imidazole interaction with the RuIIIT2 core is rationalized using energetic considerations at the quantum mechanical level of theory. 相似文献
13.
14.
Mustafa Barri George K. El Khoury Helge I. Andersson Bjrnar Pettersen 《国际流体数值方法杂志》2010,64(7):777-792
Direct numerical simulation (DNS) has been performed to study the channel flow over a backward‐facing step at a Reynolds number Reb=5600 based on the step height h and the inflow bulk velocity Ub. A dynamic method has been used in order to generate realistic turbulent inflow conditions. The results upstream of the step compared well with the fully developed channel flow. Downstream of the step our results show excellent agreement with experimental data. Copyright © 2009 John Wiley & Sons, Ltd. 相似文献
15.
Bramati A Hermier JP Khoury AZ Giacobino E Schnitzer P Michalzik R Ebeling KJ Poizat JP Grangier P 《Optics letters》1999,24(13):893-895
We studied anticorrelated quantum fluctuations between the TEM(00) and the TEM(01) transverse modes of a vertical-cavity surface-emitting semiconductor laser by measuring the transverse spatial distribution of the laser beam intensity noise. Our experimental results are found to be in good agreement with the predictions of a phenomenological model that accounts for quantum correlations between transverse modes in a light beam. 相似文献
16.
We present a nearly model-independent estimate that yields the predictions of a class of simple inflationary and ekpyrotic or cyclic models for the spectral tilt of the primordial density inhomogeneities that enables us to compare the two scenarios. Remarkably, we find that the two produce an identical result, n(s) approximately 0.95. For inflation, the same estimate predicts a ratio of tensor to scalar contributions to the low l multipoles of the microwave background anisotropy of T/S approximately 20%; the tensor contribution is negligible for ekpyrotic or cyclic models, as shown in earlier papers. 相似文献
17.
We introduce a novel two-dimensional (2D) homodyne and heterodyne technique for imaging objects through or embedded in a scattering medium. Our imaging approach is based on heterodyning of light with different Doppler broadenings that is scattered from objects of two different textures or from an opaque object and a textured scattering medium. We report on the initial demonstration of pulling signals out of noise for an object hidden behind a scattering medium. Enhancements of signal-to-noise ratio of the order of 50 have been achieved by use of a 2D holographic phase-sensitive detector. We also discuss the experimental feasibility of this approach for objects embedded in a scattering medium. 相似文献
18.
A Facile Diversity‐Oriented Multicomponent One‐Pot Synthesis of 3‐Amino‐6,7‐dihydrobenzo[c]thiophen‐4(5H)‐one Derivatives from α‐Oxo‐N,S‐ketene Acetal
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Swapnil G. Yerande Sunil D. More Mayur Bhandari Kiran M. Newase Kareem Khoury Kan Wang Alexander Dömling 《Journal of heterocyclic chemistry》2014,51(Z1):E358-E363
A convenient one‐pot multicomponent method for the preparation of 3‐amino‐6,7‐dihydrobenzo[c]thiophen‐4(5H)‐one derivative has been developed. Reaction of 1,3‐cyclohexanedione and phenyl isothiocynate gave α‐oxo‐N,S‐ketene acetal that were reacted in situ with 2‐chloromethylquniazoline‐4‐one derivatives, in the presence of sodium hydride to afford the target compound in reasonable overall yields. 相似文献
19.
Ou Z Zhu W Fang Y Sintic PJ Khoury T Crossley MJ Kadish KM 《Inorganic chemistry》2011,50(24):12802-12809
The electrochemistry of gold(III) mono- and bis-quinoxalinoporphyrins was examined in CH(2)Cl(2) or PhCN containing 0.1 M tetra-n-butylammonium perchlorate (TBAP) before and after the addition of trifluoroacetic acid to solution. The investigated porphyrins are represented as Au(PQ)PF(6) and Au(QPQ)PF(6), where P is the dianion of the 5,10,15,20-tetrakis(3,5-di-tert-butylphenyl)porphyrin and Q is a quinoxaline group fused to a β,β'-pyrrolic position of the porphyrin macrocycle; in Au(QPQ)PF(6) there is a linear arrangement where the quinoxalines are fused to pyrrolic positions that are opposite each other. The porphyrin without the fused quinoxaline groups, Au(P)PF(6), was also investigated under the same solution conditions. In the absence of acid, all three gold(III) porphyrins undergo a single reversible Au(III)/Au(II) process leading to the formation of a Au(II) porphyrin which can be further reduced at more negative potentials to give stepwise the Au(II) porphyrin π-anion radical and dianion, respectively. However, in the presence of acid, the initial Au(III)/Au(II) processes of Au(PQ)PF(6) and Au(QPQ)PF(6) are followed by an internal electron transfer and protonation to regenerate new Au(III) porphyrins assigned as Au(III)(PQH)(+) and Au(III)(QPQH)(+). Both protonated gold(III) quinoxalinoporphyrins then undergo a second Au(III)/Au(II) process at more negative potentials. The electrogenerated monoprotonated monoquinoxalinoporphyrin, Au(II)(PQH), is then further reduced to its π-anion radical and dianion forms, but this is not the case for the monoprotonated bis-quinoxalinoporphyrin, Au(II)(QPQH), which accepts a second proton and is rapidly converted to Au(III)(HQPQH)(+) before undergoing a third Au(III)/Au(II) process to produce Au(II)(HQPQH) as a final product. Thus, Au(P)PF(6) undergoes one metal-centered reduction while Au(PQ)PF(6) and Au(QPQ)PF(6) exhibit two and three Au(III)/Au(II) processes, respectively. These unusual multistep sequential Au(III)/Au(II) processes were monitored by thin-layer spectroelectrochemistry and a reduction/oxidation mechanism for Au(PQ)PF(6) and Au(QPQ)PF(6) in acidic media is proposed. 相似文献
20.
Ionic liquid glow discharge electrolysis for nanoparticle synthesis is an emerging nanomaterials processing technology and the stability of ionic liquid when they are in contact with plasma is an important issue. This paper discusses the stability of [BMIM][BF4] after exposing this ionic liquid to glow discharge plasma and the synthesis of cubic crystalline ZnS nanoparticles by plasma electrochemical method. Stability of the ionic liquid after plasma exposure to 20 min at 250 V is explained by their FTIR spectra and found that the ionic liquid is stable even after the plasma exposure. 相似文献