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Dr. Mario Leypold Lukas Schuh Prof. Roland Fischer Dr. Ana Torvisco Prof. Michaela Flock Prof. Harald Stueger Dr. Michael Haas 《Angewandte Chemie (International ed. in English)》2017,56(28):8089-8093
Herein, we report on the first sila-aldol reaction, which emphasizes the tight connection between silicon and carbon chemistry. This novel synthetic method provides straightforward access to 2-oxahexasilabicyclo[3.2.1]octan-8-ide, a structurally complex silicon framework, in quantitative yield. Its structure was confirmed by NMR spectroscopy and X-ray crystallography, and it displays a distinctive charge-transfer transition. The complete mechanism of this highly selective rearrangement cascade is outlined and supported by density functional theory (DFT) calculations, which highlight the thermodynamic driving force and the low activation barriers of this powerful silicon–carbon bond-forming strategy. 相似文献
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Michael Adamski Thomas J. G. Skalski Benjamin Britton Dr. Timothy J. Peckham Lukas Metzler Prof. Steven Holdcroft 《Angewandte Chemie (International ed. in English)》2017,56(31):9058-9061
Two classes of novel sulfonated phenylated polyphenylene ionomers are investigated as polyaromatic-based proton exchange membranes. Both types of ionomer possess high ion exchange capacities yet are insoluble in water at elevated temperatures. They exhibit high proton conductivity under both fully hydrated conditions and reduced relative humidity, and are markedly resilient to free radical attack. Fuel cells constructed with membrane-electrode assemblies containing each ionomer membrane yield high in situ proton conductivity and peak power densities that are greater than obtained using Nafion reference membranes. In situ chemical stability accelerated stress tests reveal that this class of the polyaromatic membranes allow significantly lower gas crossover and lower rates of degradation than Nafion benchmark systems. These results point to a promising future for molecularly designed sulfonated phenylated polyphenylenes as proton-conducting media in electrochemical technologies. 相似文献
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This article points at some critical issues which are connected with the theoretical formulation of the thermodynamics of
solid–fluid mixtures of frictional materials. It is our view that a complete thermodynamic exploitation of the second law
of thermodynamics is necessary to obtain the proper parameterizations of the constitutive quantities in such theories. These
issues are explained in detail in a recently published book by Schneider and Hutter (Solid–Fluid Mixtures of Frictional Materials
in Geophysical and Geotechnical Context, 2009), which we wish to advertize with these notes. The model is a saturated mixture
of an arbitrary number of solid and fluid constituents which may be compressible or density preserving, which exhibit visco-frictional
(visco-hypoplastic) behavior, but are all subject to the same temperature. Mass exchange between the constituents may account
for particle size separation and phase changes due to fragmentation and abrasion. Destabilization of a saturated soil mass
from the pre- and the post-critical phases of a catastrophic motion from initiation to deposition is modeled by symmetric
tensorial variables which are related to the rate independent parts of the constituent stress tensors. 相似文献
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Devos A Simonetti AW van der Graaf M Lukas L Suykens JA Vanhamme L Buydens LM Heerschap A Van Huffel S 《Journal of magnetic resonance (San Diego, Calif. : 1997)》2005,173(2):218-228
This study investigated the value of information from both magnetic resonance imaging and magnetic resonance spectroscopic imaging (MRSI) to automated discrimination of brain tumours. The influence of imaging intensities and metabolic data was tested by comparing the use of MR spectra from MRSI, MR imaging intensities, peak integration values obtained from the MR spectra and a combination of the latter two. Three classification techniques were objectively compared: linear discriminant analysis, least squares support vector machines (LS-SVM) with a linear kernel as linear techniques and LS-SVM with radial basis function kernel as a nonlinear technique. Classifiers were evaluated over 100 stratified random splittings of the dataset into training and test sets. The area under the receiver operating characteristic (ROC) curve (AUC) was used as a global performance measure on test data. In general, all techniques obtained a high performance when using peak integration values with or without MR imaging intensities. For example for low- versus high-grade tumours, low- versus high-grade gliomas and gliomas versus meningiomas, the mean test AUC was higher than 0.91, 0.94, and 0.99, respectively, when both MR imaging intensities and peak integration values were used. The use of metabolic data from MRSI significantly improved automated classification of brain tumour types compared to the use of MR imaging intensities solely. 相似文献
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Lukas SonnenscheinAndreas Seubert 《Tetrahedron letters》2011,52(10):1101-1104
Procedures for the synthesis of five sulfobetaine monomers as styrene derivatives are given. The five molecules form a homologous row differing in the distance between the inner quaternary amine and the outer sulfonic acid from one methylene group to five methylene groups. Syntheses are achieved by a sequence of nucleophilic substitutions starting from commercially available precursors. 相似文献