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51.
Biocatalytic Synthesis of Allylic and Allenyl Sulfides through a Myoglobin‐Catalyzed Doyle–Kirmse Reaction 下载免费PDF全文
Dr. Vikas Tyagi Dr. Gopeekrishnan Sreenilayam Dr. Priyanka Bajaj Antonio Tinoco Prof. Dr. Rudi Fasan 《Angewandte Chemie (International ed. in English)》2016,55(43):13562-13566
The first example of a biocatalytic [2,3]‐sigmatropic rearrangement reaction involving allylic sulfides and diazo reagents (Doyle–Kirmse reaction) is reported. Engineered variants of sperm whale myoglobin catalyze this synthetically valuable C?C bond‐forming transformation with high efficiency and product conversions across a variety of sulfide substrates (e.g., aryl‐, benzyl‐, and alkyl‐substituted allylic sulfides) and α‐diazo esters. Moreover, the scope of this myoglobin‐mediated transformation could be extended to the conversion of propargylic sulfides to give substituted allenes. Active‐site mutations proved effective in enhancing the catalytic efficiency of the hemoprotein in these reactions as well as modulating the enantioselectivity, resulting in the identification of the myoglobin variant Mb(L29S,H64V,V68F), which is capable of mediating asymmetric Doyle–Kirmse reactions with an enantiomeric excess up to 71 %. This work extends the toolbox of currently available biocatalytic strategies for the asymmetric formation of carbon–carbon bonds. 相似文献
52.
53.
Arjan Kuijper reas Schwarzkopf Thomas Kalbe Chandrajit Bajaj Stefan Roth & Michael Goesele 《高等学校计算数学学报(英文版)》2013,6(1):72-94
We present an efficient implementation of volumetric anisotropic image diffusion filters on
modern programmable graphics processing units (GPUs), where the mathematics behind volumetric diffusion is effectively reduced to the diffusion in 2D images.
We hereby avoid the computational bottleneck of a time consuming eigenvalue decomposition in $\mathbb{R}^3$.
Instead, we use a projection of the Hessian matrix along the surface normal onto the tangent plane of
the local isodensity surface and solve for the remaining two tangent space eigenvectors.
We derive closed formulas to achieve this and prevent the GPU code from branching.
We show that our most complex volumetric anisotropic diffusion filters gain a speed up of more than 600 compared to a CPU solution. 相似文献
54.
Nano-crystalline sulfated zirconia catalyst, prepared by two-step sol–gel method, has been studied for the solvent free self
condensation of acetophenone to dypnone. The influence of calcination temperature on the structural, textural and catalytic
activity of sulfated zirconia has been analyzed. The surface acidity along with the structural and textural features of the
catalyst influenced its activity. The conversion of acetophenone was found to be effected by the variation in the reaction
and calcination temperature, however, the dypnone selectivity was not affected much. The catalyst calcined at 650 °C, showed
maximum dypnone selectivity of 92% with 68.2% acetophenone conversion at 170 °C after 7 h. The catalyst was reused up to five
cycles with marginal decrease in acetophenone conversion, however, without losing its selectivity for dypnone. 相似文献
55.
The catalytic activity of nano-crystalline sulfated zirconia catalyst, prepared by sol–gel method and characterized by various
analytical tools, was evaluated for the esterification of caprylic acid with different short chain alcohols. The lower concentration
of catalyst (0.5 wt%) exhibited 96–98% conversion of caprylic acid with methanol and 100% selectivity for methyl caprylate
at 60 °C. The conversion was decreased with increasing carbon chain of alcohols namely with ethanol, n-propanol and n-butanol at 60 °C but increased significantly (91–98%) at higher reaction temperature. The selectivity for respective alkyl
caprylate was observed to be 100% irrespective of the alcohol used. The activity of the catalyst was slightly decreased with
successive five reaction cycles due to the water formed during the reaction. 相似文献
56.
Tamal Roy Rukhsana I. Kureshy Noor-ul H. Khan Sayed H.R. Abdi Arghya Sadhukhan Hari C. Bajaj 《Tetrahedron》2012,68(31):6314-6322
Chiral dimeric Mn(III) salen complex with 1R, 2R-(?)-diaminocyclohexane collar was immobilized on short channel large pore sized silica through a long linker of {(CH2)3–NH–melamine–piperazine} to investigate its performance in enantioselective epoxidation of chromenes, indene, styrene and cis β-methyl styrene in the presence of pyridine N-oxide (PyNO) as an axial base using aqueous NaOCl as an oxidant at 0 °C. The immobilized catalyst system showed high turnover frequency (TOF) and enantioselectivity for the smaller and bulkier alkenes like styrene, indene, 2,2-dimethylchromene and 6-cyano-2,2-dimethylchromene (ee up to 98%). These results are the best reported for heterogeneous catalyst under biphasic reaction conditions and were comparable to the dimeric Mn(III) salen system under homogeneous condition. The performance of the immobilized catalyst was retained for six reuse experiments. This protocol was extended to the synthesis of an antihypertensive drug (S)-Levchromakalim (ee 98%) at 1 g level. 相似文献
57.
Guo-lian~Xu ChandrajitL.Bajaj 《计算数学(英文版)》2003,21(5):681-688
In this paper, we provide simple and explicit formulas for computing Riemannian curvatures, mean curvature vectors, principal curvatures and principal directions for a 2-dimensional Riemannian manifold embedded in IR^k with k ≥ 3. 相似文献
58.
Reproducible improvements in the metalorganic vapor phase epitaxy (MOVPE) grown CdTe buffer quality have been demonstrated
in a horizontal rectangular duct silica reactor by the use of integratedin situ monitoring that includes laser reflectometry, pyrometry, and Epison concentration monitoring. Specular He-Ne laser reflectance
was used toin situ monitor the growth rates, layer thickness, and morphology for both ZnTe and CdTe. The substrate surface temperature was monitored
using a pyrometer which was sensitive to the 2–2.6 μm waveband and accurate to ±1°C. The group II and group VI precursor concentrations
entering the reactor cell were measured simultaneously using two Epison ultrasonic monitors and significant variations were
observed with time, in particular for DIPTe. The surface morphology and growth rates were studied as a function of VI/II ratio
for temperatures between 380 and 460°C. The background morphology was the smoothest for VI/IIratio in the vicinity of 1.5–1.75
and could be maintained using Epison monitors. Regularly shaped morphological defects were found to be associated with morphological
defects in the GaAs/Si substrate. The x-ray rocking curve widths for CuKα (531) reflections were in the range of 2.3–3.6 arc-min, with no clear trend with changing VI/II ratio. X-ray topography images
of CdTe buffer layers on GaAs/Si showed a mosaic structure that is similar to CdTe/sapphire substrates. The etch pit density
in Hg1-xCdxTe layers grown onto improved buffer layers was as low as 6 x 106 cm-2 for low temperature MOVPE growth using the interdiffused multilayer process. 相似文献
59.
Interest in the study of the behavior of shallow impurity centers in superlattices and quantum well structures is fairly recent. This paper reviews briefly both the theoretical and experimental work done in this field in the last few years. Several recent calculations of the energy levels of hydrogenic impurity states in quantum well structures, such as Ga1?xAlxAsGaAsGa1?xAlxAs, are reviewed. The behavior of these levels as a function of the quantum well size is discussed. Recent experimental data concerning the variations of the binding energies of shallow donors and acceptors as a function of the GaAs quantum well size are reviewed. A comparison between these experimental measurements and the results of recent calculations is presented. 相似文献
60.
A Case Study on the Use of Fractional Derivatives: The Low-Frequency Viscoelastic Uni-Directional Behavior of Polyurethane Foam 总被引:1,自引:0,他引:1
A fractional derivative model of dissipative effects is combined with a nonlinear elastic model to model the response of polyurethane foam in quasi-static compression tests. A system identification method is developed based on a separation of the elastic and viscoelastic parts of the response, which is possible because of symmetries in the imposed deformation time-history. Simulations are used to evaluate the proposed identification method when noise is present in the response. The system identification technique is also applied with some success to experimental data taken from several compression experiments on two types of polyurethane foam blocks. 相似文献