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1.
The oxidation of malonic acid by ceric ions has been investigated in sulfuric acid solution under a variety of conditions. The initial rate at low ceric ion concentrations is first order in each of the two reactants and has an activation energy of 11.6 kcal/mol; the instantaneous rate constant increases somewhat with time during a single run. At higher concentrations of ceric ion, semilogarithmic plots are sigmoid with a reduced rate constant at long times. The rate decreases slightly with increasing sulfuric acid concentration. Rates of carbon dioxide evolution may be much less than rates of ceric ion reduction because of supersaturation effects. The observations can be explained if dissolved oxygen reacts with organic radicals to catalyze the rate of initial attack on malonic acid, but oxygen must also be consumed irreversibly during these reactions. Computations with plausible rate constants have simulated the experimental observations. These oxygen effects can rationalize peculiar almost discontinuous changes in rate when bromomalonic acid is oxidized by ceric ion. These effects may also explain the previously puzzling observation that some Belousov–Zhabotinsky solutions are oscillatory in bulk but become quiescent but excitable when spread in a thin film in contact with air. 相似文献
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Sherrod L. MaxwellIII Brian K. Culligan Gary W. Noyes 《Journal of Radioanalytical and Nuclear Chemistry》2010,286(1):273-282
A new rapid method for the determination of actinides and radiostrontium in vegetation samples has been developed at the Savannah
River Site Environmental Lab (Aiken, SC, USA) that can be used in emergency response situations or for routine analysis. The
actinides in vegetation method utilizes a rapid sodium hydroxide fusion method, a lanthanum fluoride matrix removal step,
and a streamlined column separation process with stacked TEVA, TRU and DGA Resin cartridges. Lanthanum was separated rapidly
and effectively from Am and Cm on DGA Resin. Alpha emitters are prepared using rare earth microprecipitation for counting
by alpha spectrometry. The purified 90Sr fractions are mounted directly on planchets and counted by gas flow proportional counting. The method showed high chemical
recoveries and effective removal of interferences. The actinide and 90Sr in vegetation sample analysis can be performed in less than 8 h with excellent quality for emergency samples. The rapid
fusion technique is a rugged sample digestion method that ensures that any refractory actinide particles or vegetation residue
after furnace heating is effectively digested. 相似文献
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Sherrod L. Maxwell Brian A. Culligan Vernon D. Jones Sheldon T. Nichols Gary W. Noyes 《Journal of Radioanalytical and Nuclear Chemistry》2011,287(1):223-230
A new method that allows rapid preconcentration and separation of plutonium and neptunium in water samples was developed for the measurement of 237Np and Pu isotopes by inductively-coupled plasma mass spectrometry (ICP-MS) and alpha spectrometry. 238U can interfere with 239Pu measurement by ICP-MS as 238UH+ mass overlap and 237Np via peak tailing. The method provide enhanced removal of uranium by separating Pu and Np initially on TEVA Resin, then moving Pu to DGA resin for additional removal of uranium. The decontamination factor for uranium from Pu is almost 100,000 and the decontamination factor for U from Np is greater than 10,000. This method uses stacked extraction chromatography cartridges and vacuum box technology to facilitate rapid separations. Preconcentration is performed using a streamlined calcium phosphate precipitation method. Purified solutions are split between ICP-MS and alpha spectrometry so that long and short-lived Pu isotopes can be measured successfully. The method allows for simultaneous extraction of 20 samples (including QC samples) in 4?C6 h, and can also be used for emergency response. 239Pu, 242Pu and 237Np were measured by ICP-MS, while 236Pu, 238Pu, and 239Pu were measured by alpha spectrometry. 相似文献
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During the oxidation of carbon monoxide containing a trace of water, ten well-known atomic and molecular species can be identified as of potential significance. All conceivable reactions of these species in their ground electronic states were considered, and rate constants for all those that are of potential importance are either known or can be estimated with considerable confidence. For compositions and temperatures of experimental interest an isothermal system goes to a single steady state that is stable to perturbation and will neither explode nor oscillate. These steady-state computations also predict that as the temperature is raised above about 1000 K most of the water is converted to H, OH, and HO2 radicals. Under such conditions, exothermic reactions would be so rapid that strong thermal gradients would develop in any real system of plausible dimensions. A simple model based on these calculations predicts explosion limits consistent with those observed experimentally. Simultaneous behavior in time and in space must be calculated in detail before it is clear whether or not this model based on ground electronic states can model the oscillations that are sometimes observed in this system. 相似文献
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The oxidation of cerous ions by bromate ions in sulfuric acid medium was followed spectrophotometrically under various experimental conditions. The results were compared to the calculated predictions on the basis of a mechanism suggested by R. M. Noyes and collaborators. The computations were done by solving the complete set of the kinetic differential equations. The results of the computations show that the proposed mechanism explains adequately most of our and previous experimental data. In particular, the mechanism predicts the main features of the reaction, namely, the induction and the fast and slow reaction periods which occur during the oxidation. 相似文献
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G. Daikuhara E. Truog L. Michaelis L. T. Sharp D. R. Hoogland H. A. Noyes O. Arrhenius C. B. Lipman H. R. Christensen F. W. Parker H. Kappen A. Densch A. Rippel Th. Arnd O. Schreiner G. Loges E. Ramann F. K. Cameron R. Ulbricht W. Wolf W. Jani Biéler-Chatelan E. A. Mitscherlich C. W. Davis B. S. Davisson H. Neubauer W. Schneider Fr. Czapek G. Wunder J. K. Greisenegger K. Vorbuchner H. Niklas Hirschberger Ausschuss für Boden und Düngung des Verbandes Landwirtschaftlicher Versuchs-Stationen im Deutschen Reiche 《Analytical and bioanalytical chemistry》1924,65(6-7):273-274
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