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11.
Dr. S. James Ratnakar Dr. Sara Chirayil Dr. Alexander M. Funk Dr. Shanrong Zhang Prof. João F. Queiró Prof. Carlos F. G. C. Geraldes Prof. Zoltan Kovacs Prof. A. Dean Sherry 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(48):21855-21860
Paramagnetic chemical exchange saturation transfer (paraCEST) agents are well-suited for imaging tissue pH because the basis of CEST, chemical exchange, is inherently sensitive to pH. Several previous pH-sensitive paraCEST agents were based on an exchanging Ln3+-bound water molecule as the CEST antenna but this design often added additional line-broadening to the bulk water signal due to T2 exchange. We report herein a pH-sensitive paraCEST agent that lacks an inner-sphere water molecule but contains one Ln-bound −OH group for CEST activation. The Yb3+ complex, Yb( 1 ), displayed a single, highly shifted CEST peak originating from the exchangeable Yb-OH proton, the frequency of which changed over the biologically relevant pH range. CEST images of phantoms ranging in pH from 6 to 8 demonstrate the potential of this agent for imaging pH. Initial rodent imaging studies showed that Gd( 1 ) remains in the vascular system much longer than anticipated but is cleared slowly via renal filtration. 相似文献
12.
Junjun Wu Lu Gem Gao Zoltan Varga Xuefei Xu Wei Ren Donald G. Truhlar 《Angewandte Chemie (International ed. in English)》2020,59(27):10826-10830
Faced with the contradictory results of two recent experimental studies [Jara‐Toro et al., Angew. Chem. Int. Ed. 2017 , 56, 2166 and Chao et al., Angew. Chem. Int. Ed. 2019 , 58, 5013] of the possible catalytic effect of water vapor on CH3OH + OH reaction, we report calculations that corroborate the conclusion made by Chao et al. and extend the rate constant evaluation down to 200 K. The rate constants of the CH3OH + OH reaction catalyzed by a water molecule are computed as functions of temperature and relative humidity using high‐level electronic structure and kinetics calculations. The Wuhan–Minnesota Scaling (WMS) method is used to provide accurate energetics to benchmark a density functional for direct dynamics. Both high‐frequency and low‐frequency anharmonicities are included. Variational and tunneling effects are treated by canonical variational transition state theory with multidimensional small‐curvature tunneling. And, most significantly, we include multistructural effects in the rate constant calculations. Our calculations show that the catalytic effect of water vapor is not observable at 200–400 K. 相似文献
13.
In higher dimensional field theories with compactified dimensions there are three standard ways to do perturbative calculations: (i) by the summation over Kaluza-Klein towers; (ii) by the summation over winding numbers making use of the Poisson-resummation formula; and (iii) by using mixed propagators, where the coordinates of the four infinite dimensions are Fourier-transformed to momentum space while those of the compactified dimension are kept in configuration space. The third method is broadly used in finite temperature field theory calculations. One of its advantages is that one can easily separate the ultraviolet divergent terms of the uncompactified theory from the non-local finite corrections arising from windings around the compact dimensions. In this note we demonstrate the use of this formalism by calculating one-loop self-energy corrections in a 5D theory formulated on the manifold and on the orbifold . 相似文献
14.
15.
George Cosmin Nad Cristiana tefania Novac Ioana Adriana Matei Cosmina Maria Bouari Zoltan Miklos Gal Octavia Maria Tamas-Krumpe Adrian Maximilian Macri Nicodim Iosif Fi 《Molecules (Basel, Switzerland)》2021,26(8)
The conjunctival bacterial resident and opportunistic flora of dogs may represent a major source of dissemination of pathogens throughout the environment or to other animals and humans. Nevertheless, contamination with bacteria from external sources is common. In this context, the study of the antimicrobial resistance (AMR) pattern may represent an indicator of multidrug resistant (MDR) strains exchange. The present study was focused on a single predisposed breed—Saint Bernard. The evaluated animals were healthy, but about half had a history of ocular disease/treatment. The swabs collected from conjunctival sacs were evaluated by conventional microbiological cultivation and antimicrobial susceptibility testing (AST). The most prevalent Gram-positive was Staphylococcus spp.; regardless of the history, while Gram-negative was Pseudomonas spp.; exclusively from dogs with a history of ocular disease/treatment. Other identified genera were represented by Bacillus, Streptococcus, Trueperella, Aeromonas and Neisseria. The obtained results suggest a possible association between the presence of mixed flora and a history of ocular disease/treatment. A high AMR was generally observed (90%) in all isolates, especially for kanamycin, doxycycline, chloramphenicol and penicillin. MDR was recorded in Staphylococcus spp. and Pseudomonas spp. This result together with a well-known zoonotic potential may suggest an exchange of these strains within animal human populations and the environment. 相似文献
16.
Oxidative Conversion of a Europium(II)‐Based T1 Agent into a Europium(III)‐Based paraCEST Agent that can be Detected In Vivo by Magnetic Resonance Imaging 下载免费PDF全文
Dr. Alexander M. Funk Dr. Veronica Clavijo Jordan Prof. A. Dean Sherry Dr. S. James Ratnakar Prof. Zoltan Kovacs 《Angewandte Chemie (International ed. in English)》2016,55(16):5024-5027
The EuII complex of 1,4,7,10‐tetraazacyclododecane‐1,4,7,10‐tetraacetic acid (DOTA) tetra(glycinate) has a higher reduction potential than most EuII chelates reported to date. The reduced EuII form acts as an efficient water proton T1 relaxation reagent, while the EuIII form acts as a water‐based chemical exchange saturation transfer (CEST) agent. The complex has extremely fast water exchange rate. Oxidation to the corresponding EuIII complex yields a well‐defined signal from the paraCEST agent. The time course of oxidation was studied in vitro and in vivo by T1‐weighted and CEST imaging. 相似文献
17.
Meija J Mester Z D'Ulivo A 《Journal of the American Society for Mass Spectrometry》2006,17(7):1028-1036
Three conceptually different mathematical methods are presented for accurate mass spectrometric determination of H2O/HOD/D2O and H2Se/HDSe/D2Se concentrations from mixtures. These are alternating least-squares, weighted two-band target entropy minimization, and a statistical mass balance model. The otherwise nonmeasurable mass spectra of partially deuterated isotopologues (HOD and HDSe) are mathematically constructed. Any recorded isotopologue mixture mass spectra are then deconvoluted by least-squares into their components. This approach is used to study the H2O/D2O exchange reaction, and is externally validated gravimetrically. The H2O/D2O exchange equilibrium constant is also measured from the deconvoluted 70 eV electron impact GC/MS data (K = 3.85 +/- 0.03). 相似文献
18.
Addition of a benzyl substituent to the macrocyclic ring of DOTA has a substantial impact on the conformational ring flipping motion of the macrocycle in the resulting LnDOTA complexes. The p-NO2-benzyl substituent in the Ln(p-NO2-Bn-DOTA)- complexes lies in an equatorial position and effectively "locks" the conformation of the ring into the deltadeltadeltadelta configuration. The presence of the p-NO2-benzyl group also increases the population of the square antiprismatic (SAP) coordination isomer for all Ln(p-NO2-Bn-DOTA)- complexes relative to that seen for the respective LnDOTA- complexes. Despite this increase in SAP isomer population, the rate of water exchange in these complexes remains comparatively fast. The kinetic and thermodynamic stabilities of the Ln(p-NO2-Bn-DOTA)- complexes are also slightly lower than the corresponding LnDOTA- complexes but appear to be sufficiently high for in vivo use. 相似文献
19.
In Vivo Endoscopic Tissue Identification by Rapid Evaporative Ionization Mass Spectrometry (REIMS) 下载免费PDF全文
Dr. Julia Balog Dr. Sacheen Kumar James Alexander Ottmar Golf Dr. Juzheng Huang Tom Wiggins Nima Abbassi‐Ghadi Dr. Attila Enyedi Dr. Sandor Kacska James Kinross Prof. George B. Hanna Prof. Jeremy K. Nicholson Prof. Zoltan Takats 《Angewandte Chemie (International ed. in English)》2015,54(38):11059-11062
Gastrointestinal cancers are a leading cause of mortality, accounting for 23 % of cancer‐related deaths worldwide. In order to improve outcomes from these cancers, novel tissue characterization methods are needed to facilitate accurate diagnosis. Rapid evaporative ionization mass spectrometry (REIMS) is a technique developed for the in vivo classification of human tissue through mass spectrometric analysis of aerosols released during electrosurgical dissection. This ionization technique was further developed by utilizing surface induced dissociation and was integrated with an endoscopic polypectomy snare to allow in vivo analysis of the gastrointestinal tract. We tested the classification performance of this novel endoscopic REIMS method in vivo. It was shown to be capable of differentiating between healthy layers of the intestinal wall, cancer, and adenomatous polyps based on the REIMS fingerprint of each tissue type in vivo. 相似文献
20.
Zoltan Bajko Dietrich Gudat Falk Lissner Martin Nieger Thomas Schleid 《无机化学与普通化学杂志》2004,630(12):1969-1976
Phosphonio‐benzo[c]phospholides with an additional phosphonium ylide substituent in 3‐position were synthesized by deprotonation of appropriately substituted 1, 3‐bis‐phosphonio benzophospholide cations and characterized by spectroscopic and analytical data. The ability of these molecules to act as bidentate P, C‐chelating ligands to transition metal atoms was demonstrated in the reactions with [W(CO)4(norbornadiene)] and [MCl2(cyclooctadiene)] (M = Pd, Pt). The PdII and PtII complexes are distinguished by a strong inclination towards addition of H2O to the 10π‐electron system of the ligand. The molecular structures of a W0 complex with a P, C‐chelating ylidyl‐phosphonio‐benzophospholide ligand and of the product resulting from H2O‐addition to a corresponding PtII complex were determined. The structural parameters of the W0 complex provide evidence for the presence of substantial steric strain around the metal atom. 相似文献