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991.
Bassarello C Cimino P Bifulco G Boger DL Smith JA Chazin WJ Gomez-Paloma L 《Chembiochem : a European journal of chemical biology》2003,4(11):1188-1193
We report the NMR solution structure of (+)-CPI-indole (CPI, 1,2,8,8a-tetrahydrocyclopropa[c]pyrrolo[3,2-e]indol-4(5H)-one), an agent belonging to the CC-1065/duocarmycin family of antitumor compounds. This (+)-CPI-indole structure is covalently bound to d(G(1)ACTAATTGTC(11))-d(G(12)TCAATTAGTC(22)), a synthetic DNA duplex containing a high-affinity binding site. The three-dimensional structure has been determined by several cycles of restrained molecular dynamics calculations with a total of 563 NMR-derived constraints, both in vacuo and by using the generalized Born solvent continuum model. In-depth analysis of the structure of this ligand-DNA complex led to a detailed knowledge of the bound state conformation of the CPI-indole, the most simplified agent related to CC-1065 and duocarmycins, the parent members of a family of extremely potent antitumor compounds. Comparison of the CPI-indole bound conformation with those previously found for (+)-duocarmycin SA (DSA), its unnatural enantiomer (-)-DSA, and the demethoxylated analogue (+)-DSI in their DNA complexes provided additional evidence of the tight correlation between the catalytic effect exerted by DNA on the alkylation reaction and the extent of angular twist between the two planar heteroaromatic subunits of these agents. Additionally, comparison of the structural features of the DNA-bound state of a "naked" ligand, such as CPI-indole, with those of various other duocarmycin agents provided useful information for the interpretation of the observed effects on chemical reactivity of the different substitution patterns at the hemispheres of these types of complex. 相似文献
992.
Escaja N Gómez-Pinto I Rico M Pedroso E González C 《Chembiochem : a European journal of chemical biology》2003,4(7):623-632
The structures and stabilities of cyclic DNA octamers of different sequences have been studied by NMR and CD spectroscopy and by restrained molecular dynamics. At low oligonucleotide concentrations, some of these molecules form stable monomeric structures consisting of a short stem of two base pairs connected by two mini-loops of two residues. To our knowledge, these dumbbell-like structures are the smallest observed to date. The relative stabilities of these cyclic dumbbells have been established by studying their melting transitions. Dumbbells made up purely of GC stems are more stable than those consisting purely of AT base pairs. The order of the base pairs closing the loops also has an important effect on the stabilities of these structures. The NMR data indicate that there are significant differences between the solution structures of dumbbells with G-C base pairs in the stem compared to those with A-T base pairs. In the case of dumbbells with G-C base pairs, the residues in the stem form a short segment of a BDNA helix stabilized by two Watson-Crick base pairs. In contrast, in the case of d, the stem is formed by two A-T base pairs with the glycosidic angles of the adenine bases in a syn conformation, most probably forming Hoogsteen base pairs. Although the conformations of the loop residues are not very well defined, the thymine residues at the first position of the loop are observed to fold back into the minor groove of the stem. 相似文献
993.
M. Abdelaziz 《应用聚合物科学杂志》2004,94(5):2178-2186
Poly(vinyl alcohol) (PVA) films filled with (x)CsBr(15 ? x)MnCl2, where 0.0 ≤ x ≤ 15%, were prepared by a casting technique. The crystal structure properties of the prepared films were examined by XRD, DTA, and FTIR. A correlation between XRD, DTA, and FTIR of the filled polymer was discussed. Optical absorption measurements revealed two optical band gaps (Eg1 and Eg2). The electrical properties were studied using dc electrical conductivity. The filling level (FL) dependency of Eg1 and Eg2, thermal activation energy (ΔE), and hopping distance (R0) are given to illustrate the behavior of the filled polymers. © 2004 Wiley Periodicals, Inc. J Appl Polym Sci 94: 2178–2186, 2004 相似文献
994.
Achim Feldermann 《Polymer》2004,45(12):3997-4007
Reversible addition fragmentation chain transfer (RAFT) mediated and conventional copolymerizations at low monomer conversions have been carried out for the systems methyl methacrylate (MMA)-styrene, methyl acrylate (MA)-styrene and methyl methacrylate-butyl acrylate (BA). The polymer samples have been analyzed via 1H-NMR spectroscopy to obtain the copolymer composition and the terminal model reactivity ratios. In the RAFT mediated copolymerizations, the polymer mole fraction of the monomer with the larger reactivity ratio is increased compared to the conventional copolymerization. Simulations have been carried out using the program package PREDICI® to examine possible explanations for the experimental findings. The simulations demonstrate that the RAFT process itself may alter the macroradical populations and the copolymer composition by offering additional reaction pathways. Further, the rate coefficients for the initiation reaction and the pre-equilibrium play an important role in determining the copolymer composition. The rate coefficients governing the main equilibrium of the RAFT process have only a minor impact on the copolymer composition. 相似文献
995.
A new material, which can be used in solar energy utilization, is obtained here by adding different weights of poly(vinyl alcohol) (PVA) to the semiconducting material CdS. The effect of this addition was studied by using FT‐Raman spectrometer (based on 1500 mW Nd : YAG laser at 1064 nm), UV–Vis‐IR (190–800 nm) spectrophotometer, and X‐ray diffractometer. Our experimental results indicated the appearance of several new Raman bands, which have not existed in both CdS and PVA. Some of the bands which are already existing in the Raman spectra of PVA showed an unexpected systematic increase in their intensities after the addition of CdS to the matrix. On the other hand, some of the new Raman bands appeared in special concentrations of PVA only, whereas some of the Raman bands of CdS were found to disappear after adding PVA. Finally, shifts in some bands associated with random increase in their intensities after adding PVA to CdS was detected in the FT‐Raman analysis. The experimental evidence given here might be attributed to the occurrence of new bonds, indicating that the produced mixture is a new material. The assignment of the new bands as well as an interpretation of the obtained variations is given here. Our X‐ray diffraction data confirmed the interpretation introduced here. Moreover, the UV–Vis spectra confirmed the existence of new absorption bands in the Visible region. The I‐V characteristic curve was measured for a selected concentration of the new composite material, showing a remarkable increase in the values of the conduction current of about two orders of magnitude as compared with the pure PVA material. © 2004 Wiley Periodicals, Inc. J Appl Polym Sci 92: 1984–1992, 2004 相似文献
996.
A neural network is trained to estimate the unknown crystallinity and temperature of Nylon 6 and its nanocomposites while the material is undergoing cooling at a fixed rate. The innovation of the work is that the full spectrum captured by the laser Raman spectroscope is used to train a neural network for estimation of crystallinity and temperature. The small‐angle light scattering (SALS) and differential scanning calorimetry (DSC) data were used to provide the training examples for the neural network. Results indicate that the neural network can provide reliable estimates of the crystallinity and temperature provided that there is a sufficient number of training data available. Neural network methodology is also efficient in establishing the crystallization–temperature relationship as a function of cooling rate and demonstrates the heterogeneous nucleation effect of nanoclay in the nylon 6 matrix. © 2004 Wiley Periodicals, Inc. J Appl Polym Sci 92: 474–483, 2004 相似文献
997.
Poly(methylphenylene) (PMeP) films were prepared by direct oxidation of toluene in the mixed electrolytes of boron trifluoride diethyl etherate (BFEE) and trifluoroacetic acid (TFA). The oxidation potential of toluene in pure BFEE was measured to be 1.52 V versus saturated calomel electrode (SCE). This value was much lower than that determined in a neutral medium such as acetonitrile (2.13 V versus SCE). The introduction of TFA into BFEE decreased the oxidation potential of toluene and also improved the properties of as‐formed polymer films. Infrared and Raman spectra confirmed the formation of PMeP films. © 2004 Wiley Periodicals, Inc. J Appl Polym Sci 93: 189–195, 2004 相似文献
998.
A. P. Kharitonov Yu. L. Moskvin D. A. Syrtsova V. M. Starov V. V. Teplyakov 《应用聚合物科学杂志》2004,92(1):6-17
Fluorinated polymers have a set of unique properties, including improved chemical stability and thermal stability and good barrier and membrane parameters, which are mainly defined by their surface properties. This article presents systematic data on the direct fluorination of the polyimide Matrimid® 5218, a commercially available polymer suitable for the formation of gas‐separation hollow fibers. Changing the fluorination conditions (i.e., the fluorinated mixture composition, fluorine partial pressure, and treatment duration) allows the rate of formation of the surface‐fluorinated layer over the 0.1–10 μm range to be kept under control. The physicochemical properties of modified layers (i.e., the chemical composition, formation of radicals, refractive index, IR and UV spectra, density, and surface energy) are examined. The thickness of the fluorinated layer (δF) depends on the fluorination duration (t): δF ~ t0.5. During fluorination, hydrogen atoms are replaced with fluorine, double bonds are saturated with fluorine, and at least one CN bond in the five‐member ring is disrupted. Fluorination results in a significant increase in the polymer density, transparency in the visible and ultraviolet regions of spectra, and a reduction of the refractive index. A high concentration of long‐living radicals (up to ~5 × 1019 radicals/cm3 of the fluorinated layer) is generated under fluorination. This can be used for subsequent grafting (e.g., with acrylonitrile). © 2004 Wiley Periodicals, Inc. J Appl Polym Sci 92: 6–17, 2004 相似文献
999.
Infrared (IR) spectroscopy studies were performed for poly(methyl methacrylate) (PMMA) samples doped with an organic ligand or its cobalt(II) complex after the extraction of the dopant during γ‐radiolysis. There were no drastic changes in the IR absorption band position, but noticeable changes in the intensities were found. The relative transmission of IR absorption bands, such as those at 750, 840, 1065, and 1388 cm?1, were measured according to the transmission of the carbonyl group band at 1717 cm?1. The degradation and recombination mechanism of different groups in the polymeric chain or backbone during radiolysis could be explained by the behavior of the relative transmission data for each group with increasing exposure dose. The tacticity of the PMMA samples was unchanged during radiolysis, and they were found to be syndiotactic. This was confirmed by the IR J values for different PMMA samples before and after irradiation. The protection efficiency of the organic ligand and its cobalt(II) complex was also investigated, and it was found that the organic ligand was more protective than the cobalt(II) complex for PMMA samples against γ‐rays. © 2003 Wiley Periodicals, Inc. J Appl Polym Sci 91: 1937–1950, 2004 相似文献
1000.