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Cody Ross Pitts Michelle Sheanne Bloom Desta Doro Bume Qinze Arthur Zhang Thomas Lectka 《Chemical science》2015,6(9):5225-5229
Expanding the repertoire of controlled radical fluorination techniques, we present a photosensitized unstrained C–C bond activation/directed monofluorination method using Selectfluor and 9-fluorenone. The reaction is amenable to the opening of multiple 1-acetal-2-aryl substituted rings to yield ω-fluoro carboxylic acids, esters, alcohols, and ketones with relative ease. Initial mechanistic insight suggests radical ion intermediates. 相似文献
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Ingrida Steponavičė Rob J. Hyndman Kate Smith-Miles Laura Villanova 《Journal of Global Optimization》2017,67(1-2):263-282
This paper presents a meta-algorithm for approximating the Pareto optimal set of costly black-box multiobjective optimization problems given a limited number of objective function evaluations. The key idea is to switch among different algorithms during the optimization search based on the predicted performance of each algorithm at the time. Algorithm performance is modeled using a machine learning technique based on the available information. The predicted best algorithm is then selected to run for a limited number of evaluations. The proposed approach is tested on several benchmark problems and the results are compared against those obtained using any one of the candidate algorithms alone. 相似文献
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Hydroxylation of the silica in microfabricated thin layer chromatography plates as probed by time‐of‐flight secondary ion mass spectrometry and diffuse reflectance infrared Fourier transform spectroscopy 下载免费PDF全文
Supriya S. Kanyal Bhupinder Singh Cody V. Cushman Daniel T. Jankowski Matthew R. Linford 《Surface and interface analysis : SIA》2015,47(3):340-344
Microfabricated silica thin layer chromatography (TLC) plates have previously been prepared on patterned carbon nanotube forests. The high temperatures used in their fabrication reduce the number of hydroxyl groups on their surfaces. Fortunately, silica can be rehydroxylated. In diffuse reflectance infrared Fourier transform spectroscopy (DRIFT), a silanol peak below 3740 cm?1 indicates a well‐hydroxylated silica surface that is fit for chromatography. Hydroxylations of our materials with HF are so effective that it is not possible to discern the position of this peak. In contrast, this signal is discernable when the plates are treated with NH4OH. To find a more convenient method for studying the surfaces of TLC plates, time‐of‐flight secondary ion mass spectroscopy (ToF‐SIMS) was considered. ToF‐SIMS is advantageous because multiple microfabricated TLC plates must be scraped to obtain enough silica for one DRIFT analysis, while static SIMS can be performed on very small regions (500 × 500 µm2 or less) of individual plates. Ratios of the SiOH+ and Si+ ToF‐SIMS signals for microfabricated TLC plates correlated well with ~3740 cm?1 silanol peaks from DRIFT. Thus, SIMS allows direct analysis of all of our treated and untreated plates, including those hydroxylated with HF. The best hydroxylation condition for HF, which was better than any studied for NH4OH, was around 150 ppm at room temperature. The best hydroxylation condition for NH4OH was 50 °C for 72 h. ToF‐SIMS versus DRIFT results of commercial TLC plates were also obtained and evaluated. Copyright © 2014 John Wiley & Sons, Ltd. 相似文献
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We provide explicit solutions of certain forward-backward stochastic differential equations (FBSDEs) with quadratic growth. These particular FBSDEs are associated with quadratic term structure models of interest rates and characterize the zero-coupon bond price. The results of this paper are naturally related to similar results on affine term structure models of Hyndman (Math. Financ. Econ. 2(2):107–128, 2009) due to the relationship between quadratic functionals of Gaussian processes and linear functionals of affine processes. Similar to the affine case a sufficient condition for the explicit solutions to hold is the solvability in a fixed interval of Riccati-type ordinary differential equations. However, in contrast to the affine case, these Riccati equations are easily associated with those occurring in linear-quadratic control problems. We also consider quadratic models for a risky asset price and characterize the futures price and forward price of the asset in terms of similar FBSDEs. An example is considered, using an approach based on stochastic flows that is related to the FBSDE approach, to further emphasize the parallels between the affine and quadratic models. An appendix discusses solvability and explicit solutions of the Riccati equations. 相似文献
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Prof. Li Chen Genevieve E. Mullen Myriam Le Roch Cody G. Cassity Prof. Nicolas Gouault Prof. Henry Y. Fadamiro Prof. Robert E. Barletta Prof. Richard A. O'Brien Prof. Richard E. Sykora Prof. Alexandra C. Stenson Prof. Kevin N. West Howard E. Horne Jeffrey M. Hendrich Kang Rui Xiang Prof. James H. Davis Jr. 《Angewandte Chemie (International ed. in English)》2014,53(44):11762-11765
The practical utility of ionic liquids (ILs) makes the absence (heretofore) of reported examples from nature quite puzzling, given the facility with which nature produces many other types of exotic but utilitarian substances. In that vein, we report here the identification and characterization of a naturally occurring protic IL. It can be formed during confrontations between the ants S. invicta and N. fulva. After being sprayed with alkaloid‐based S. invicta venom, N. fulva detoxifies by grooming with its own venom, formic acid. The mixture is a viscous liquid manifestly different from either of the constituents. Further, we find that the change results as a consequence of formic acid protonation of the N centers of the S. invicta venom alkaloids. The resulting mixed‐cation ammonium formate milieu has properties consistent with its classification as a protic IL. 相似文献
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Yuetian Yan Masaaki Ubukata Robert B. Cody Timothy E. Holy Michael L. Gross 《Journal of the American Society for Mass Spectrometry》2014,25(8):1404-1411
A method for structural elucidation of biomolecules dating to the 1980s utilized high-energy collisions (~10 keV, laboratory frame) that induced charge-remote fragmentations (CRF), a class of fragmentations particularly informative for lipids, steroids, surfactants, and peptides. Unfortunately, the capability for high-energy activation has largely disappeared with the demise of magnetic sector instruments. With the latest designs of tandem time-of-flight mass spectrometers (TOF/TOF), however, this capability is now being restored to coincide with the renewed interest in metabolites and lipids, including steroid-sulfates and other steroid metabolites. For these metabolites, structure determinations are required at concentration levels below that appropriate for NMR. To meet this need, we explored CRF with TOF/TOF mass spectrometry for two groups of steroid sulfates, 3-sulfates and 21-sulfates. We demonstrated that the current generation of MALDI TOF/TOF instruments can generate charge-remote fragmentations for these materials. The resulting collision-induced dissociation (CID) spectra are useful for positional isomer differentiation and very often allow the complete structure determination of the steroid. We also propose a new nomenclature that directly indicates the cleavage sites on the steroid ring with carbon numbers. Figure
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