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Dr. Ruth Matesanz Dr. José Fernando Diaz Dr. Francisco Corzana Andrés G. Santana Dr. Agatha Bastida Dr. Juan Luis Asensio 《Chemistry (Weinheim an der Bergstrasse, Germany)》2012,18(10):2875-2889
The most common mode of bacterial resistance to aminoglycoside antibiotics is the enzyme‐catalysed chemical modification of the drug. Over the last two decades, significant efforts in medicinal chemistry have been focused on the design of non‐ inactivable antibiotics. Unfortunately, this strategy has met with limited success on account of the remarkably wide substrate specificity of aminoglycoside‐modifying enzymes. To understand the mechanisms behind substrate promiscuity, we have performed a comprehensive experimental and theoretical analysis of the molecular‐recognition processes that lead to antibiotic inactivation by Staphylococcus aureus nucleotidyltransferase 4′(ANT(4′)), a clinically relevant protein. According to our results, the ability of this enzyme to inactivate structurally diverse polycationic molecules relies on three specific features of the catalytic region. First, the dominant role of electrostatics in aminoglycoside recognition, in combination with the significant extension of the enzyme anionic regions, confers to the protein/antibiotic complex a highly dynamic character. The motion deduced for the bound antibiotic seem to be essential for the enzyme action and probably provide a mechanism to explore alternative drug inactivation modes. Second, the nucleotide recognition is exclusively mediated by the inorganic fragment. In fact, even inorganic triphosphate can be employed as a substrate. Third, ANT(4′) seems to be equipped with a duplicated basic catalyst that is able to promote drug inactivation through different reactive geometries. This particular combination of features explains the enzyme versatility and renders the design of non‐inactivable derivatives a challenging task. 相似文献
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Bharat Kumar Ruth L. Viboh Margel C. Bonifacio William B. Thompson Jonathan C. Buttrick Babe C. Westlake Min‐Soo Kim Robert W. Zoellner Sergey A. Varganov Philipp Mrschel Jaroslav Teteruk Martin U. Schmidt Benjamin T. King 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2012,124(51):13071-13071
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Morgan and Culler proved that a minimal action of a free group on a tree is determined by its translation length function. We prove an analogue of this theorem for 2-dimensional right-angled Artin groups acting on CAT(0) rectangle complexes. 相似文献
46.
Sean A.C. McDowell C. Ruth Le Sueur A. David Buckingham Anthony J. Stone 《Molecular physics》2013,111(5):823-835
The integrated intensities of vibrational transitions depend on the magnitude of the derivatives of the dipole with respect to nuclear motion. Normally, the only reliable way to compute such derivatives is by tedious and expensive ab initio calculations. In this paper, we present a simplification for weakly bound complexes based on distributed schemes for describing the charge densities and polarizabilities of the monomers. Formulations based on both Cartesian and spherical harmonics are presented. The results for both these schemes agree exactly with each other, and qualitatively with full ab initio calculations for the hydrogen fluoride dimer, (HF)2. 相似文献
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Mihály V. Pilipecz Tamás R. Varga Péter Králl Zoltán Vincze Zoltán Mucsi Ruth Deme 《合成通讯》2020,50(11):1712-1723
AbstractThe novel push–pull alkene, the 2-(nitro-nitrosomethylene)-pyrrolidine with numerous aliphatic or aromatic amines as nucleophiles afforded amidoximes. Various substituted oxadiazaborole and oxadiazole derivatives were prepared starting from these amidoximes, widening the synthetic applicability of the push–pull alkenes. Acylation of the amidoximes was also examined. The mechanism of the amidoxime formation was investigated by computational methods. 相似文献
48.
Franziska Pecho Dr. You-Quan Zou Johannes Gramüller Prof. Dr. Tadashi Mori Prof. Dr. Stefan M. Huber Dr. Andreas Bauer Prof. Dr. Ruth M. Gschwind Prof. Dr. Thorsten Bach 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(23):5190-5194
A chiral phosphoric acid with a 2,2’-binaphthol core was prepared that displays two thioxanthone moieties at the 3,3’-position as light-harvesting antennas. Despite its relatively low triplet energy, the phosphoric acid was found to be an efficient catalyst for the enantioselective intermolecular [2+2] photocycloaddition of β-carboxyl-substituted cyclic enones (e.r. up to 93:7). Binding of the carboxylic acid to the sensitizer is suggested by NMR studies and by DFT calculations to occur by means of two hydrogen bonds. The binding event not only enables an enantioface differentiation but also modulates the triplet energy of the substrates. 相似文献
49.
Alberto Blzquez-Moraleja Ines Senz-de-Santa María María D. Chiara Delia lvarez-Fernndez Inmaculada García-Moreno Ruth Prieto-Montero Virginia Martínez-Martínez Iigo Lpez Arbeloa Jose Luis Chiara 《Chemical science》2020,11(4):1052
The first fluorescent probes that are actively channeled into the mitochondrial matrix by a specific mitochondrial membrane transporter in living cells have been developed. The new functional probes (BCT) have a minimalist structural design based on the highly efficient and photostable BODIPY chromophore and carnitine as a biotargeting element. Both units are orthogonally bonded through the common boron atom, thus avoiding the use of complex polyatomic connectors. In contrast to known mitochondria-specific dyes, BCTs selectively label these organelles regardless of their transmembrane potential and in an enantioselective way. The obtained experimental evidence supports carnitine–acylcarnitine translocase (CACT) as the key transporter protein for BCTs, which behave therefore as acylcarnitine biomimetics. This simple structural design can be readily extended to other structurally diverse starting F-BODIPYs to obtain BCTs with varied emission wavelengths along the visible and NIR spectral regions and with multifunctional capabilities. BCTs are the first fluorescent derivatives of carnitine to be used in cell microscopy and stand as promising research tools to explore the role of the carnitine shuttle system in cancer and metabolic diseases. Extension of this approach to other small-molecule mitochondrial transporters is envisaged.A BODIPY derivative of carnitine enters mitochondria regardless of their membrane potential and in an enantioselective way through a specific mitochondrial membrane transporter in living cells. 相似文献
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