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1.
The heterogeneous enantioselective hydrogenation of activated ketones over chirally modified platinum is reviewed with emphasis on identifying the role of the various species observed in this catalytic system. The past years have witnessed a continuous broadening of the scope of this catalytic system including new reactants and modifiers affording over 97% ee. New reaction pathways have been uncovered and the kinetic and mechanistic studies have been faced with a number of complicating factors caused by spectator species and interactions in solution and on the Pt surface. The previously proposed mechanistic models are critically assessed in the light of these new findings. 相似文献
2.
By comparing the experimental data of the Sauter-mean-diameter d 32 and the hold up ? with models from literature, there are presented equations for d 32 and ? for the used conical turbine in gas-liquid systems. The necessary adjustment of the proportionality constants of the literature equations will be explained on the basis of fluiddynamical phenomena. It can be established by fluid-dynamical results of a former study carried out with laser-doppler-anemometry. Coalescence phenomena are taken into account in the model using an analogy to bubble columns. The analogy to bubble columns turns out to be suitable. Arguments for the necessity of considering the local fluiddynamics in the modelling of dispersions are presented. 相似文献
3.
An anomalous rate enhancement with increasing conversion has been observed during the liquid phase hydrogenation of nitrobenzene and crotonaldehyde over Ge/Pd/C catalysts at ambient temperature and atmospheric pressure. Inductive coupled plasma atomic emission spectroscopy and electrochemical measurement of the oxidation state of catalysts during reaction revealed that the bimetallic particles were partially oxidized by the reactants, which resulted in Ge-dissolution and increased exposure of Pd on the surface. It is proposed that the surface and bulk composition of Ge/Pd catalysts are a function of their oxidation state. This behaviour is due to the unusually high mobility of Ge in the Pd lattice and to the good solubility of GeO2 in polar solvents. The influence of hydrogen transport on the corrosion process and the stability of other X/Pd type bimetallic catalysts during liquid phase hydrogenation are also discussed. 相似文献
4.
Thomas Bürgi Fachri Atamny Axel Knop‐Gericke Michael Hävecker Thomas Schedel‐Niedrig Robert Schlögl Alfons Baiker 《Catalysis Letters》2000,66(3):109-112
The adsorption of ethyl pyruvate on Pt(111) has been studied by in situ XANES measurements in the presence and absence of
hydrogen. Depending on the hydrogen and ethyl pyruvate pressure, the C and O K‐edge spectra exhibit distinctly different angular
dependence. Without hydrogen ethyl pyruvate is oriented preferentially perpendicular to the surface, indicating bonding via
the O lone pairs. In the presence of hydrogen the mean orientation is more tilted towards the surface. Likely, ethyl pyruvate
also interacts with Pt via its π system under these conditions. The observed angle‐dependent shift of the energy of the π*
and σ* resonances indicates the coexistence of differently adsorbed ethyl pyruvate species. The experimental findings demonstrate
the importance of the in situ approach for unraveling the adsorption mode of ethyl pyruvate in the enantioselective hydrogenation
over cinchona‐alkaloid‐modified Pt.
This revised version was published online in July 2006 with corrections to the Cover Date. 相似文献
5.
Anna Puig-Molina Lars Pleth Nielsen Alfons M. Molenbroek Konrad Herbst 《Catalysis Letters》2004,92(1-2):29-34
The chemical state of arsenic deposited on a NiMoP/Al2O3 hydrotreating catalyst exposed to ppb levels of arsenic over several years in a refinery reactor has been studied by in situ EXAFS. In the as-received As-NiMoP catalyst, arsenic is exclusively coordinated to oxygen atoms. Upon sulfiding the sample in 2%H2S/2%H2/96%He, the As atoms become surrounded by approximately two sulfur atoms. No evidence was found for Ni–As bond formation. A possible model for the As local environment is suggested on the basis of combined EXAFS results, STM data and FEFF8.0 simulations (program for ab initio calculations on multiple scattering XAFS and XANES). The FEFF8.0 simulations of the proposed model are in accord with the experimental data measured at the As K edge. In this model, an As atom is located at the edge of a hexagonally truncated Ni-MoS2 slab and is blocking the active NiMoS site. 相似文献
6.
A model system for the study of structural and chemical properties of monolayers and multilayers of vanadium oxide immobilized on titania is presented. Investigation of the planar oxide-oxide interface by XP, UV and IS spectroscopy indicated that vanadium immobilized by a single impregnation step exists as an incomplete heterogeneous layer containing well dispersed V4+ species. Increase of the vanadia loading by multiple impregnations led to vanadia agglomerates with higher apparent oxidation state of the vanadium. TD spectroscopy with O2 and CO2 as probe molecules revealed that the chemical reactivity of the vanadia surface species depends on their structure. The surface containing well-dispersed vanadia species exchanged oxygen more easily and showed pronounced interactions with CO2. 相似文献
7.
Maria Casapu Jan-Dierk Grunwaldt Marek Maciejewski Meike Wittrock Ulrich Gbel Alfons Baiker 《Applied catalysis. B, Environmental》2006,63(3-4):232-242
The formation and stability of BaAl2O4 and BaCeO3 in Pt-Ba/Al2O3 and Pt-Ba/CeO2 based NOx storage-reduction (NSR) catalysts has been investigated using kinetic measurements, X-ray diffraction, thermal analysis and X-ray absorption spectroscopy. In as-prepared state, the Ba-component in the NSR catalysts was made up of amorphous BaO and BaCO3. The formation of BaAl2O4 started above 850 °C, whereas the formation of BaCeO3 was already observed at 800 °C and was faster than that of BaAl2O4. The stability of BaAl2O4 and BaCeO3 in various liquid and gaseous atmospheres was different. BaAl2O4 was rapidly hydrated at room temperature in the presence of water and transformed to Ba(NO3)2 and γ-alumina in the presence of HNO3, whereas BaCeO3 was decomposed to much lower extent under these conditions. Interestingly, BaCeO3 was transformed to Ba(NO3)2/CeO2 in the presence of NO2/H2O at 300–500 °C. Also, the presence of CO2 led to decomposition of barium cerate, which has important consequences for the catalyst ageing under NOx-storage conditions and can be exploited for regeneration of thermally aged NSR-catalysts. 相似文献
8.
Pt–Ba/MeO (where MeO = Al2O3, CeO2, SiO2 and ZrO2) NO
x
storage-reduction catalysts with Ba-loading varying from 0 wt.% to 28 wt.% were investigated concerning stability of Ba phases
and NO
x
storage-reduction efficiency. For Pt–Ba/Al2O3 three different Ba-containing phases with different thermal stability are distinguished based on their interaction with the
support. The relative concentration of these phases varies with the Ba-loading and NO
x
storage tests indicated that the BaCO3 phase decomposing between 400 °C and 800 °C (LT-BaCO3) is the most efficient Ba containing phase for NO
x
storage. Similar investigations of Pt–Ba catalysts supported on CeO2, SiO2 and ZrO2 showed that the relative amount of LT-BaCO3 phase depends also on the support material. NO
x
storage measurements confirmed a correlation between the concentration of LT-BaCO3 and NO
x
storage efficiency. Basicity and textural properties of the support are identified as crucial parameters for efficient NO
x
storage catalysts. 相似文献
9.
10.
Dynamic memory allocation has been used for decades. However, it has seldom been used in real-time systems since the worst
case of spatial and temporal requirements for allocation and deallocation operations is either unbounded or bounded but with
a very large bound.
In this paper, a new allocator called TLSF (Two Level Segregated Fit) is presented. TLSF is designed and implemented to accommodate
real-time constraints. The proposed allocator exhibits time-bounded behaviour, O(1), and maintains a very good execution time. This paper describes in detail the data structures and functions provided by
TLSF. We also compare TLSF with a representative set of allocators regarding their temporal cost and fragmentation.
Although the paper is mainly focused on timing analysis, a brief study and comparative analysis of fragmentation incurred
by the allocators has been also included in order to provide a global view of the behaviour of the allocators.
The temporal and spatial results showed that TLSF is also a fast allocator and produces a fragmentation close to that caused
by the best existing allocators.
相似文献
Alfons Crespo (Corresponding author)Email: |