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11.
Carmen L. Huffman Melissa Lee Williams D. Michelle Benoist Richard E. Overstreet Emily E. Jellen‐McCullough 《Rapid communications in mass spectrometry : RCM》2011,25(16):2299-2306
In collision‐induced dissociation mass spectrometry experiments, the collision energy required for dissociation linearly depends on the degrees of freedom in the precursor ion. The magnitude of the slope of this relationship previously has been shown to qualitatively correlate to the relative binding strength of a noncovalently bound, monovalent complex. The goal of the work presented here is to determine if a similar methodology can be applied for assessing relative binding strengths in multivalent species. We have tested the method on complexes formed from 18‐crown‐6 and a variety of protonated, primary alkylamines, [CnH2n+1NH3]+ (n = 9, 12, 14, 16 and 18) and alkyldiamines, [H3NCnH2nNH3]2+ (n = 3, 5, 6, 9 and 12), and compared our results with dissociation energies calculated using density functional theory at the B3LYP/6‐31G* level. We found that the method correctly assessed the stronger crown ether/headgroup interaction in the two divalent species (1:1 and 2:1 complexes formed from the diaminoalkanes) compared with the weaker interaction in the monovalent species (1:1 complexes formed from mono‐aminoalkanes). However, the experimental method could not distinguish between the binding strengths of the two divalent complexes, perhaps because their calculated dissociation energies were quite similar. Our preliminary results suggest that this method could potentially be used for a quick and simple analysis of binding strengths in multivalent species if the binding strengths of the species are significantly different from one another. Copyright © 2011 John Wiley & Sons, Ltd. 相似文献
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Melting temperatures were observed visually for poly-(2,6-dimethyl-1,4-phenylene oxide) in methylene chloride at nine concentrations (polymer weight fractions ranging from 0.0042 to 0.2362). The data were analyzed upon the assumptions that ΔHu and ΔSu, the molar heat and entropy of fusion per polymer unit, are constant over the temperature range studied, and that a Flory-Huggins chemical potential expression with a concentration-independent pair interaction parameter, χ1 = (0.5 + ψ1) + ψ1Φ/T, satisfactorily describes the polymer unit activity in the binary solutions. Computation gave ΔHu = 1404 cal/mole of units (therefore Δh = 11.7 cal/g), ψ1 = ?0.5691, and Φ = 342.4°K. The effect of using various combinations of data points upon the values of these three parameters, as determined by least-squares linear regression treatment of the melting temperature expression, is indicated. 相似文献
14.
The free-volume theory for the temperature dependence of transport properties of glass-forming polymers is extended to obtain their relationship to the extent of cure. This treatment centers on the unifying role of molecular mobility and yields a model which connects extent of reaction, viscosity, diffusivity, ionic conductivity and dipole relaxation time. The temporal dependence of these properties is expressed by coupling the extended free-volume model with a relationship for the rate of cure, which included diffusional limitations. Analyses based on this model are applied to the observed behavior of a model epoxy-amine resin system. The intrinsic kinetics of this model system are shown to be first order. It is shown that diffusional limitations strongly affected the progress of the reaction in the final stages of cure. The diffusion-modified rate expression predictions agree with extent of reaction versus time data over the range of experimental temperatures. The temporal dependence of viscous behavior of the curing resin is measured. The extended free-volume model accurately describes the evolution of resin viscosity during cure. The dielectric behavior is similarly characterized and is in close agreement with the predictions of the general free-volume expression. The results of this study indicate that the free-volume theory modified to account for molecular weight effects allows prediction of resin properties with a two-parameter model. The results show that a power-law relationship exists between viscosity and ionic conductivity. This result suggests that electrical properties may be used for on-line measurement of resin viscosity during cure. 相似文献
15.
A micro-interferometric technique for measuring out-of-plane thermal displacements on a scale commensurate with the dimensions of the fiber/matrix unit cell is described. A scanning micro-interferometer is used to image surface displacements of samples containing a single-pitch-based carbon fiber embedded in an epoxy matrix. The interferometer design gives the necessary resolution to detect small changes in thermal displacements in the fiber/matrix interface region. The samples were heated electrically through the fiber to create radially symmetric temperature and displacement fields. Repeatable displacement measurements were obtained on a radial line across the interface region with an accuracy of ±25 Å. A sharp expansion of the matrix surrounding the fiber was observed with each heating. Overall, the experiments demonstrate the utility of micro-interferometry for measuring submicron displacements. 相似文献
16.
J. Glister G. Ron B.W. Lee R. Gilman A.J. Sarty S. Strauch D.W. Higinbotham E. Piasetzky K. Allada W. Armstrong J. Arrington H. Arenhövel A. Beck F. Benmokhtar B.L. Berman W. Boeglin E. Brash A. Camsonne J. Calarco J.P. Chen S. Choi E. Chudakov L. Coman B. Craver F. Cusanno J. Dumas C. Dutta R. Feuerbach A. Freyberger S. Frullani F. Garibaldi J.-O. Hansen T. Holmstrom C.E. Hyde H. Ibrahim Y. Ilieva C.W. de Jager X. Jiang M.K. Jones Hyekoo Kang A. Kelleher E. Khrosinkova E. Kuchina G. Kumbartzki J.J. LeRose R. Lindgren P. Markowitz S. May-Tal Beck E. McCullough D. Meekins 《Physics letters. [Part B]》2011
17.
An action of a finite group on a closed 2-manifold is called almost free if it has a single orbit of points with nontrivial stabilizers. It is called large when the order of the group is greater than or equal to the genus of the surface. We prove that the orientation-preserving large almost free actions of G on closed orientable surfaces correspond to the Nielsen equivalence classes of generating pairs of G . We classify the almost free actions on the surfaces of genera 3 and 4, find the large almost free actions of the alternating group A5, and give various other examples. 相似文献
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Evaluating the accuracy of theoretical one‐bond 13C─13C scalar couplings and their ability to predict structure in a natural product
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Jacob Powell Domenic Valenti Harley Bobnar Erika Drain Blaine Elliott Sydney Frank Tyler McCullough Sean Moore Andrew Kettring Robbie Iuliucci James K. Harper 《Magnetic resonance in chemistry : MRC》2017,55(11):979-989
This study explores the feasibility of using a combination of experimental and theoretical 1‐bond 13C─13C scalar couplings (1JCC) to establish structure in organic compounds, including unknowns. Historically, nJCC and nJCH studies have emphasized 2 and 3‐bond couplings, yet 1JCC couplings exhibit significantly larger variations. Moreover, recent improvements in experimental measurement and data processing methods have made 1JCC data more available. Herein, an approach is evaluated in which a collection of theoretical structures is created from a partial nuclear magnetic resonance structural characterization. Computed 1JCC values are compared to experimental data to identify candidates giving the best agreement. This process requires knowledge of the error in theoretical methods, thus the B3LYP, B3PW91, and PBE0 functionals are evaluated by comparing to 27 experimental values from INADEQUATE. Respective errors of ±1.2, ±3.8, and ±2.3 Hz are observed. An initial test of this methodology involves the natural product 5‐methylmellein. In this case, only a single candidate matches experimental data with high statistical confidence. This analysis establishes the intramolecular hydrogen‐bonding arrangement, ring heteroatom identity, and conformation at one position. This approach is then extended to hydroheptelidic acid, a natural product not fully characterized in prior studies. The experimental/theoretical approach proposed herein identifies a single best‐fit structure from among 26 candidates and establishes, for the first time, 1 configuration and 3 conformations to complete the characterization. These results suggest that accurate and complete structural characterizations of many moderately sized organic structures (<800 Da) may be possible using only 1JCC data. 相似文献
20.
Darryl McCullough 《Mathematische Zeitschrift》1990,205(1):421-436
Supported in part by the National Science Foundation 相似文献