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61.
Paulo A. Machicao Scott R. Burt Ryan K. Christensen Nathan B. Lohner J.D. Singleton Matt A. Peterson 《Tetrahedron letters》2017,58(24):2318-2321
Treatment of N-[(4-hydroxy-6-phenyl)pyrimidin-2-yl]cyanamide with 1° alkyl or arylamines in isopropyl alcohol for only 10 min at 110–120 °C under microwave conditions gave the corresponding N′-alkyl(aryl)guanidine derivatives in excellent yields (65–84%). Isolated yields were greatest when >1.0 equiv. of amines were employed, but excellent results were also obtained when aryl and alkylamines were reacted with a more atom-economical loading (1.0 equiv.; 70% and 72% ave. yields, respectively). Arylamines with either highly electron withdrawing substituents (e.g. CO2H) or pi-deficient heterocycles (e.g. variously substituted aminopyridines) did not work well under these conditions, and reaction with ureas and/or amino acids did not give detectable products. Work-up was exceedingly simple, and involved simple collection and washing of product on a sintered glass funnel. Products were obtained in analytically pure form and required approximately 1 h to prepare, start to finish. 相似文献
62.
Sémeril D Matt D Toupet L Oberhauser W Bianchini C 《Chemistry (Weinheim an der Bergstrasse, Germany)》2010,16(46):13843-13849
The two rhodium complexes [Rh(acac)(L(R))] (L(R)=(S,S)-5,11,17,23-tetra-tert-butyl-25,27-di(OR)-26,28-bis(1,1'-binaphthyl-2,2'-dioxyphosphanyloxy)calix[4]arene; 6: R=benzyl, 7: R=fluorenyl), each based on a hemispherical chelator forming a pocket about the metal centre upon chelation, are active in the hydroformylation of 1-octene and styrene. As expected for this family of diphosphanes, both complexes resulted in remarkably high selectivity towards the linear aldehyde in the hydroformylation of 1-octene (l/b≈15 for both complexes). Linear aldehyde selectivity was also observed when using styrene, but surprisingly only 6 displayed a marked preference for the linear product (l/b=12.4 (6) vs. 1.9 (7)). A detailed study of the structure of the complexes under CO or CO/H(2) in toluene was performed by high-pressure NMR (HP NMR) and FT-IR (HP-IR) spectroscopies. The spectroscopic data revealed that treatment of 6 with CO gave [Rh(acac)(CO)(η(1)-L(benzyl))] (8), in which the diphosphite behaves as a unidentate ligand. Subsequent addition of H(2) to the solution resulted in a well-defined chelate complex with the formula [RhH(CO)(2)(L(benzyl))] (9). Unlike 6, treatment of complex 7 with CO only led to ligand dissociation and concomitant formation of [Rh(acac)(CO)(2)], but upon addition of H(2) a chelate complex analogous to 9 was formed quantitatively. In both [RhH(CO)(2)(L(R))] complexes the diphosphite adopts the bis-equatorial coordination mode, a structural feature known to favour the formation of linear aldehydes. As revealed by variable-temperature NMR spectroscopy, these complexes show the typical fluxionality of trigonal bipyramidal [RhH(CO)(2)(diphosphane)] complexes. The lower linear selectivity of 7 versus 6 in the hydroformylation of styrene was assigned to steric effects, due to the pocket in which the catalysis takes place being less adapted to accommodate CO or larger olefins and, therefore, possibly leading to facile ligand decoordination. This interpretation was corroborated by an X-ray structure determination carried out for 7. 相似文献
63.
International Intercomparison of Solar UVR Spectral Measurement Systems in Melbourne in 2013
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Peter Gies Rebecca Hooke Richard McKenzie John O'Hagan Stuart Henderson Andy Pearson Marina Khazova John Javorniczky Kerryn King Matt Tully Michael Kotkamp Bruce Forgan Stephen Rhodes 《Photochemistry and photobiology》2015,91(5):1237-1246
Monitoring ambient solar UVR levels provides information on how much there is in both real time and historically. Quality assurance of ambient measurements of solar UVR is critical to ensuring accuracy and stability and this can be achieved by regular intercomparisons of spectral measurement systems with those of other organizations. In October and November of 2013 a solar UVR spectroradiometer from Public Health England (PHE) was brought to Melbourne for a campaign of intercomparisons with a new Bentham spectrometer of Australian Radiation Protection and Nuclear Safety Agency (ARPANSA) and one at the Australian Bureau of Meteorology (BOM), supported by New Zealand's National Institute for Water and Atmosphere (NIWA). Given all three spectroradiometers have calibrations that are traceable to various national standards, the intercomparison provides a chance to determine measurement uncertainties and traceability that support UV measurement networks in Australia, New Zealand and the UK. UV Index measurements from all three systems were compared and ratios determined for clear sky conditions when the scans from each instrument were within 2 min of each other. While wavelengths below 305 nm showed substantial differences between the PHE unit and the two other systems, overall the intercomparison results were encouraging, with mean differences in measured UV Index between the BOM/NIWA and those of PHE and ARPANSA of <0.1% and 7.5%, respectively. 相似文献
64.
Matt Taddy 《Journal of computational and graphical statistics》2017,26(3):525-536
The statistics literature of the past 15 years has established many favorable properties for sparse diminishing-bias regularization: techniques that can roughly be understood as providing estimation under penalty functions spanning the range of concavity between ?0 and ?1 norms. However, lasso ?1-regularized estimation remains the standard tool for industrial Big Data applications because of its minimal computational cost and the presence of easy-to-apply rules for penalty selection. In response, this article proposes a simple new algorithm framework that requires no more computation than a lasso path: the path of one-step estimators (POSE) does ?1 penalized regression estimation on a grid of decreasing penalties, but adapts coefficient-specific weights to decrease as a function of the coefficient estimated in the previous path step. This provides sparse diminishing-bias regularization at no extra cost over the fastest lasso algorithms. Moreover, our gamma lasso implementation of POSE is accompanied by a reliable heuristic for the fit degrees of freedom, so that standard information criteria can be applied in penalty selection. We also provide novel results on the distance between weighted-?1 and ?0 penalized predictors; this allows us to build intuition about POSE and other diminishing-bias regularization schemes. The methods and results are illustrated in extensive simulations and in application of logistic regression to evaluating the performance of hockey players. Supplementary materials for this article are available online. 相似文献
65.
In this paper, we give a direct construction for a set of dice realizing any given tournament T. The construction for a tournament with n vertices requires dice with n sides if n is odd, sides if n is divisible by 4, and sides if mod 4. This appears to be the most efficient general construction to date. Our construction relies only on a standard construction from graph theory. 相似文献
66.
67.
We show that any k-fold covering using translates of an arbitrary convex polygon can be decomposed into Ω(k) covers. Such a decomposition can be computed using an efficient (polynomial-time) algorithm. 相似文献
68.
Chaofeng Zhang Matt Quince Zhixin Chen Zaiping Guo Huakun Liu 《Journal of Solid State Electrochemistry》2011,15(11-12):2645-2652
In this work, the potential of using coconut shell, which is very cheap and readily available, for the production of graphitic nanocarbon three-dimensional networks is investigated. The three-dimensional carbon has been produced via the wet-impregnation of coconut shell powder with a transition metal catalyst. The novel process employed offers low costs and environmental advantages, with biological waste used in place of carbonaceous precursor as the feedstock. Nanocarbon/tin oxide composites were prepared via wet-impregnation and the solvothermal method, using tin chloride solution with the activated nanocarbon. The electrochemical performances of the three-dimensional nanocarbon doped with tin oxide and of activated nanocarbon alone as anode materials were investigated in rechargeable lithium ion batteries. One composite made by using the solvothermal method shows stable cyclic retention up to 100 cycles and delivers a high reversible capacity of about 405?mAh g?1. 相似文献
69.
Mohammad Reza Yaftian Saeed Rayati Daryoush Emadi Dominique Matt 《Analytical sciences》2006,22(8):1075-1078
The preparation of a lead-selective electrode based on 5,11,17,23-tetra-tert-butyl-25,26,27,28-tetrakis-(diphenylphosphinoylmethoxy)calix[4]arene (1) as an ionophore is reported. The plasticized PVC membrane containing 30% PVC, 57% ortho-nitrophenyloctylether (NPOE), 4% sodium tetraphenylborate (NaTPB) and 9% ionophore 1 was directly coated on a graphite electrode. It exhibits a nearly Nernstian slope of 28.0 +/- 0.2 mV decade(-1) over a concentration range of 1 x 10(-5) - 1 x 10(-2) mol dm(-3) with a detection limit of 1.4 x 10(-6) mol dm(-3). The response time of the electrode was found to be ca. 17 s. The potential of the sensor was independent of the pH variation in the range 3.5 - 5.0. The selectivity of the electrode performance towards lead ions over Th4+, La3+, Sm3+, Dy3+, Y3+, Ca2+, Sr2+, Cd2+, Mn2+, Zn2+, Ni2+, Co2+, NH4+ Ag+, Li+, Na+ and K+ ions was investigated. The prepared electrode was used successfully as an indicator electrode for a potentiometric titration of a lead solution using a standard solution of EDTA. The applicability of the sensor for Pb2+ measurements in various synthetic water samples spiked with lead nitrate was also checked. 相似文献
70.
Matt J. Kipper Soenke Seifert P. Thiyagarajan Balaji Narasimhan 《Journal of Polymer Science.Polymer Physics》2005,43(5):463-477
Synchrotron small‐angle X‐ray scattering (SAXS) was used to study the isothermal crystallization kinetics of a family of polyanhydride copolymers consisting of 1,6‐bis(p‐carboxyphenoxy)hexane and sebacic acid monomers. In situ SAXS experiments permitted the direct observation of the crystallization kinetics. The structural parameters (the long period, lamellar thickness, and degree of crystallinity) were obtained from Lorentz‐corrected intensity profiles, one‐dimensional correlation functions, and interface distribution functions to form a comprehensive picture of the crystal morphology. The combination of these three analyses provided information not only on the lamellar dimensions but also on the polydispersity (nonuniformity) of these dimensions. Where possible, the crystallization kinetics were interpreted with a modified version of the Avrami equation. The results can be used to perform the rational design of controlled‐drug‐release formulations because crystallinity affects drug‐release kinetics. © 2005 Wiley Periodicals, Inc. J Polym Sci Part B: Polym Phys 43: 463–477, 2005 相似文献