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431.
Amos B. Smith III Chris Sfouggatakis Christina A. Risatti Jeffrey B. Sperry Wenyu Zhu Victoria A. Doughty Takashi Tomioka Dimitar B. Gotchev Clay S. Bennett Satoshi Sakamoto Onur Atasoylu Shohei Shirakami David Bauer Makoto Takeuchi Jyunichi Koyanagi Yasuharu Sakamoto 《Tetrahedron》2009,65(33):6489-5984
Three syntheses of the architecturally complex, cytotoxic marine macrolide (+)-spongistatin 1 (1) are reported. Highlights of the first-generation synthesis include: use of a dithiane multicomponent linchpin coupling tactic for construction of the AB and CD spiroketals, and their union via a highly selective Evans boron-mediated aldol reaction en route to an ABCD aldehyde; introduction of the C(44)-C(51) side chain via a Lewis acid-mediated ring opening of a glucal epoxide with an allylstannane to assemble the EF subunit; and final fragment union via Wittig coupling of the ABCD and EF subunits to form the C(28)-C(29) olefin, followed by regioselective Yamaguchi macrolactonization and global deprotection. The second- and third-generation syntheses, designed with the goal of accessing 1 g of (+)-spongistatin 1 (1), maintain both the first-generation strategy for the ABCD aldehyde and final fragment union, while incorporating two more efficient approaches for construction of the EF Wittig salt. The latter combine the original chelation-controlled dithiane union of the E- and F-ring progenitors with application of a highly efficient cyanohydrin alkylation to append the F-ring side chain, in conjunction with two independent tactics to access the F-ring pyran. The first F-ring synthesis showcases a Petasis-Ferrier union/rearrangement protocol to access tetrahydropyrans, permitting the preparation of 750 mg of the EF Wittig salt, which in turn was converted to 80 mg of (+)-spongistatin 1, while the second F-ring strategy, incorporates an organocatalytic aldol reaction as the key construct, permitting completion of 1.009 g of totally synthetic (+)-spongistatin 1 (1). A brief analysis of the three syntheses alongside our earlier synthesis of (+)-spongistatin 2 is also presented. 相似文献
432.
433.
Hydrogen from Formic Acid through Its Selective Disproportionation over Sodium Germanate—A Non‐Transition‐Metal Catalysis System
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Dr. Ruth I. J. Amos Dr. Falk Heinroth Dr. Bun Chan Sisi Zheng Prof. Brian S. Haynes Prof. Christopher J. Easton Prof. Anthony F. Masters Prof. Leo Radom Prof. Thomas Maschmeyer 《Angewandte Chemie (International ed. in English)》2014,53(42):11275-11279
A robust catalyst for the selective dehydrogenation of formic acid to liberate hydrogen gas has been designed computationally, and also successfully demonstrated experimentally. This is the first such catalyst not based on transition metals, and it exhibits very encouraging performance. It represents an important step towards the use of renewable formic acid as a hydrogen‐storage and transport vector in fuel and energy applications. 相似文献
434.
A formal total synthesis of (−)-brevisamide has been achieved. The synthetic approach highlights a chemoselective asymmetric dihydroxylation and a one-pot Fraser-Reid epoxidation/PMB protection reaction sequence. 相似文献
435.
Summary.
With denoting the -th partial
sum of ${\rm e}^{z}$, the exact rate of convergence of the zeros of the
normalized partial sums, , to the Szeg\"o curve
was
recently studied by Carpenter et al. (1991), where
is defined by
Here, the above results are generalized to the convergence of
the zeros and poles of certain sequences of normalized Pad\'{e}
approximants
to , where is the associated Pad\'{e} rational approximation to .
Received February 2, 1994 相似文献
436.
Tom van Dijk Dr. Sebastian Burck Amos J. Rosenthal Dr. Martin Nieger Dr. Andreas W. Ehlers Dr. J. Chris Slootweg Prof. Dr. Koop Lammertsma 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(26):9328-9331
Iminophosphanes are a new group of 1,3‐P,N‐ligands, readily obtainable from secondary phosphanes and nitrilium ions, having a tunable N‐donor site by means of varying the imine substituents. These ligands give, in high yields, monodentate gold complexes and bidentate rhodium and iridium complexes. Crystal structures are reported for both the ligands and the complexes. 相似文献
437.
Titanium dioxide was deposited from aqueous suspension onto cellulosic surfaces.Titania was sourced from Degussa (P25TM,70:30 anatase:rutile).Dry uptake of particles was shown to be rapid and dominant with one-third of the deposition occurring in less than 30 s and over one-half in the first minute.Isotherms were recorded to compare the rate of titanium deposition on dry and pre-wetted cotton.In the dry case uptake reached a maximum in 30 min whereas in the pre-wetted case the uptake was seen to continue beyond 180 min.A broad trend of higher deposition occurring at lower pH was seen,corresponding to the region where surface charges were opposite and thus attractive.Dry pickup was less significant at high pH.The response to varying ionic strength was complex and was attributed to the combined effect of charge screening,particle aggregation and consequent particle entrapment or occlusion.Titania deposition into the interstices of woven cotton sheets resulted in the formation of inorganic,nanoparticulate skeletons which could be isolated by controlled combustion of the cellulose and thus cotton was suggested to have potential for the templated synthesis of high surface area semiconductor materials. 相似文献
438.
439.
The differential elastic scattering cross-sections of intermediate energy antiprotons from Carbon and Aluminum have been analysed to determine parameter values of analytic representations of the optical model, distorted waves; such representations being convenient for use in analyses of non elastic reaction data. 相似文献
440.
Regulation of glucose carriers in chick fibroblasts 总被引:3,自引:0,他引:3