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1.
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
2.
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
3.
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
4.
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
5.
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
6.
We have developed an episomal replicating expression vector in which the SV40 gene coding for the large T-antigen was replaced by chromosomal scaffold/matrix attached regions. Southern analysis as well as vector rescue experiments in CHO cells and in Escherichia coli demonstrate that the vector replicates episomally in CHO cells. It occurs in a very low copy number in the cells and is stably maintained over more than 100 generations without selection pressure. 相似文献
7.
Platinum deposited onto high and low surface area graphites are used as model catalysts in studying the irreversible catalyst
deactivation observed previously in the aerobic oxidation of L-sorbose to 2-keto-L-gulonic acid. The corrosion of platinum
in the neutral aqueous solution was followed in the liquid cell of a scanning tunnelling microscope. Leaching of platinum
was well detectable in the time scale of 1-2 h. Depending on the nature of graphite support and the Pt content, a considerable
fraction or even all Pt dissolved during sorbose oxidation, as evidenced by cyclic voltammetry. The strikingly high rate of
Pt dissolution into the neutral aqueous medium under ambient conditions is attributed to the excellent chelating properties
of the polyhydroxy carboxylic acid product.
This revised version was published online in July 2006 with corrections to the Cover Date. 相似文献
8.
9.
H Baiker 《Canadian Metallurgical Quarterly》1976,101(42):1545-1546
10.
Robert Büchel Reto Strobel Alfons Baiker Sotiris E. Pratsinis 《Topics in Catalysis》2009,52(13-20):1799-1802
High surface area Pt/K/Al2O3 catalysts were prepared with a 2-nozzle flame spray method resulting in Pt clusters on γ-Al2O3 and amorphous K storage material as evidenced by Raman spectroscopy. The powders had a high NO x storage capacity and were regenerated fast in a model exhaust gas environment. From 300 to 400 °C no excess NO x was detected in the off gas during transition from fuel lean to fuel rich conditions, resulting in a highly effective NO x removal performance. Above 500 °C, the NSR activity was lost and not recovered at lower temperatures as K-compounds were partially crystallized on the catalyst. 相似文献