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181.
Mohammed I. Jeraal Nicholas Holmes Geoffrey R. Akien Richard A. Bourne 《Tetrahedron》2018,74(25):3158-3164
Reaction optimisation and understanding is fundamental for process development and is achieved using a variety of techniques. This paper explores the use of self-optimisation and experimental design as a tandem approach to reaction optimisation. A Claisen-Schmidt condensation was optimised using a branch and fit minimising algorithm, with the resulting data being used to fit a response surface model. The model was then applied to find new responses for different metrics, highlighting the most important for process development purposes. 相似文献
182.
(±)β-Vetivone and (±) 10-epi-β-vetivone have been synthesized in 6 steps via an efficient spiroannelation-functionalization sequence. 相似文献
183.
184.
McLain Derek R. Brossard Tom W. Tsai Yifen Condon Nicholas J. Canaday Jodi L. 《Journal of Radioanalytical and Nuclear Chemistry》2022,331(5):2169-2174
Journal of Radioanalytical and Nuclear Chemistry - Two methods were used to evaluate the age of 75Se sealed source material. Both methods utilized gamma spectroscopy to determine the quantity of... 相似文献
185.
Nicholas Favalli Gabriele Bassi Tania Zanetti Jrg Scheuermann Dario Neri 《Helvetica chimica acta》2019,102(4)
The construction of DNA‐encoded chemical libraries (DECLs) crucially relies on the availability of chemical reactions, which are DNA‐compatible and which exhibit high conversion rates for a large number of diverse substrates. In this work, we present our optimization and validation procedures for three copper and palladium‐catalyzed reactions (Suzuki cross‐coupling, Sonogashira cross‐coupling, and copper(I)‐catalyzed alkyne‐azide cycloaddition (CuAAC)), which have been successfully used by our group for the construction of large encoded libraries. 相似文献
186.
Nicholas J. Race Qianjia Yuan Prof. Matthew S. Sigman 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(2):512-515
A palladium-catalyzed enantioselective redox-relay Heck reaction of 2-indole triflates and disubstituted alkenes is reported. This process combines readily available indole triflates with a variety of alkenes to afford a range of indole derivatives bearing a stereocenter adjacent to C2. Enantioselectivity is achieved through use of a simple pyridine-oxazoline ligand. Tuning the electronics of the indole, through judicious choice of N-protecting group, is required to ensure selective β-hydride elimination away from the indole core. Utility of this method is highlighted in a modular formal synthesis of an S1P1 agonist precursor developed by Merck. 相似文献
187.
Yunhua Chen Nicholas Ballard Oliver D. Coleman Ian J. Hands‐Portman Stefan A. F. Bon 《Journal of polymer science. Part A, Polymer chemistry》2014,52(12):1745-1754
We demonstrate that the volume phase transition temperature (VPTT) of copolymer microgel particles made from N‐isopropylacrylamide (NIPAm) and methacryloyl hydrazide (MH) can be tailored in a reversible manner upon the reaction of the hydrazide functional groups with aldehydes. The microgels were synthesized by precipitation polymerization in water. Due to the water‐soluble nature of the MH monomer, the VPTT at which the microgel particles contract shifts to higher values by increasing the incorporated amounts of methacryloyl hydrazide from 0 to 5.0 mol %. The VPTT of the copolymer microgel dispersions in water can be fine‐tuned upon addition of hydrophobic/hydrophilic aldehydes, which react with the hydrazide moiety to produce the hydrazone analogue. This hydrazone formation is reversible, which allows for flexible, dynamic control of the thermo‐responsive behavior of the microgels. The ability to “switch” the VPTT was demonstrated by exposing hydrophilic streptomycin sulfate salt incubated microgel particles to an excess of a hydrophobic aldehyde, that is benzaldehyde. The temperature at which these microgels contracted in size upon heating was markedly lowered in these aldehyde exchange experiments. Transformation into benzaldehyde hydrazone derivatives led to assembly of the microgel particles into small colloidal clusters at elevated temperatures. This control of supracolloidal cluster formation was also demonstrated with polystyrene particles which had a hydrazide functionalised microgel shell. © 2014 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2014 , 52, 1745–1754 相似文献
188.
Ganyuan Xiao Dr. James R. D. Montgomery Dr. Christopher S. Lancefield Dr. Isabella Panovic Prof. Dr. Nicholas J. Westwood 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(54):12397-12402
Selective processing of the β-O-4 unit in lignin is essential for the efficient depolymerisation of this biopolymer and therefore its successful integration into a biorefinery set-up. An approach is described in which this unit is modified to incorporate a carboxylic ester with the goal of enabling the use of mild depolymerisation conditions. Inspired by preliminary results using a Cu/TEMPO/O2 system, a protocol was developed that gave the desired β-O-4-containing ester in high yield using certain dimeric model compounds. The optimised reaction conditions were then applied to an oligomeric lignin model system. Extensive 2D NMR analysis demonstrated that analogous chemistry could be achieved with the oligomeric substrate. Mild depolymerisation of the ester-containing oligomer delivered the expected aryl acid monomer. 相似文献
189.
In the game of cops and robber, the cops try to capture a robber moving on the vertices of the graph. The minimum number of cops required to win on a given graph G is called the cop number of G. The biggest open conjecture in this area is the one of Meyniel, which asserts that for some absolute constant C, the cop number of every connected graph G is at most . In a separate paper, we showed that Meyniel's conjecture holds asymptotically almost surely for the binomial random graph. The result was obtained by showing that the conjecture holds for a general class of graphs with some specific expansion‐type properties. In this paper, this deterministic result is used to show that the conjecture holds asymptotically almost surely for random d‐regular graphs when d = d(n) ≥ 3. 相似文献
190.
A Roe‐type decomposition for a system of equations governing onshore/offshore wave transformation in coastal waters is derived. The equation set approximated pertains to coastal waters prior to wave breaking, and is based on depth‐averaging and time‐averaging of the Euler equations. The equations are those used in many commercial codes for simulation of wave height and wave‐averaged currents. This novel approach uses a combination of some standard Roe averages, together with physical reasoning and power series expansions to derive a Roe‐averaged Jacobian (with real, linearly independent eigenvectors) and ensures conservation, and thereby effects the decomposition. It is shown that the resulting derived Roe‐averaged quantities are accurate to a high degree, by comparing them with their analytical equivalents for a wide range of nondimensional water depths and slopes likely to be encountered in coastal problems. Numerical tests of time‐invariant wave height transformation and wave group propagation are undertaken; these indicate good performance of the scheme in practice. Copyright © 2011 John Wiley & Sons, Ltd. 相似文献