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71.
K. Juodkazis J. Juodkazyt? T. Juodien? V. Šukien? I. Savickaja 《Electrochimica acta》2006,51(27):6159-6164
The idea of underpotential oxidation of water, taking place on the surface of noble metals in the range of potentials preceding molecular oxygen evolution, is more than 40-years old. Chemisorbed oxygen atom—Ochem is considered to be the main intermediate in the underpotential oxidation of H2O, leading eventually to chemical oxidation of noble metals and formation of anhydrous surface oxides of MeO type. This concept is still used for the evaluation of the real surface area of the noble metal electrodes and also for the interpretation of new experimental results.The existence of reversible metal-oxide electrodes demonstrated experimentally for Pt, Pd, Rh, Ir and Au electrodes, oxidized anodically in the range of potentials preceding O2 evolution, shows that noble metals do have electrochemistry of their own. Nanometric layers of amorphous, slightly soluble hydroxides, hydrous oxides or oxides can form electrochemically on the electrode surface during the anodic process and be reduced during the cathodic one. Such alternative concept admits the reversibility of anodic and cathodic processes and changes essentially the understanding and interpretation of the phenomena of anodic oxidation of noble metals. 相似文献
72.
Mesoporous molecular sieve MCM-41 with a Si/Al ratio of 35 was obtained by hydrothermal synthesis using a gel mixture with a molar composition of 6 SiO20.1 Al2O31 hexadecyltrimethylammonium chloride 0.25 dodecyltrimethylammonium bromide 0.25 tetrapropylammonium bromide0.15 (NH4)2O1.5 Na2O300 H2O. The MCM-41 sample was calcined in O2 flow at 813 K and subsequently ion exchanged with Ca2+. A small Pt cluster has been supported on the MCM-41 sample following a procedure using ion exchange of Pt(NH3)
4
2+
. The Pt(NH3)
4
2+
ion supported on MCM-41 has been activated in O2 flow at 593 K and subsequently reduced with Fh flow at 573 K, in the same way used for the preparation of a Pt cluster entrapped inside the supercage of zeolite NaY. The resulting Pt cluster supported on the MCM-41 shows hydrogen chemisorption oftotal two H atoms per Pt at 296 K (based on the total amount of Pt) and high catalytic activity for hydrogenolysis of ethane. The chemical shift in129Xe NMR spectroscopy of adsorbed xenon indicates that the Pt cluster is located inside the mesoporous molecular sieve. 相似文献
73.
Chanho Pak Seung Jae Lee Seol-Ah Lee Hyuk Chang 《Korean Journal of Chemical Engineering》2005,22(2):214-218
To reduce the effect of methanol permeated from the anode, the structure of the cathode was modified from a single layer with
Pt black catalyst to two-layer with PtRh black and Pt black catalysts, respectively. The current density of the direct methanol
fuel cell (DMFC) using the two-layer cathode was improved to 228 mA/cm-2 compared to that (180 mA/cm-2) of the DMFC using the single layer cathode at 0.3 V and 303 K. From the cyclic voltammograms (CVs), it is indicated that
the amount of adsorbates on the metal catalyst in the two-layer cathode is less than that of adsorbates in the single layer
cathode after methanol test. In addition, the adsorbates were removed very rapidly by electrochemical oxidation from the two-layer
cathode. It is suggested fromex situ X-ray absorption near edge structure analysis that the d-electron vacancy of Pt atom in the two-layer cathode is not changed
by the methanol test. Thus, Pt is not covered with the adsorbates, which agrees well with the results of CV. 相似文献
74.
A catalyst for NOx storage/reduction was prepared to improve the activity of Ba–Pt/γ-Al2O3 by replacing Ba with a mixture of Ba and Mg. The catalyst was prepared by impregnating Pt and then co-impregnating Ba and
Mg (Mg:Ba molar ratio = 1) on commercial γ-Al2O3. The tests have been carried out in the presence of CO2 at temperatures between 200 and 400 °C in order to understand the role of both the feed and various alkaline-earth metals.
The storage capacity of the two catalysts was different like the mechanism in the reduction process. 相似文献
75.
A. Goifman J. Gun V. Gitis A. Kamyshny Jr. O. Lev J. Donner H. Brnick E. Worch 《Applied catalysis. B, Environmental》2004,54(4):225-235
Pyrolysed carbon supported cobalt porphyrin, an electrocatalyst that is frequently used for oxygen reduction in fuel cells, is evaluated for catalytic oxidation of hydrogen sulfide by dissolved dioxygen. The catalyst performs best after heat treatment at 880 °C, at pH 8. Analysis of the reaction products reveals that sulfur is the dominant product throughout the investigated pH range 5–10. The catalyst performs much better than powdered activated carbon, granular activated carbon and different other forms of unmodified carbon catalysts. This is as far as we know the first time that heat treated cobalt porphyrins are evaluated for non-electrocatalytic applications. 相似文献
76.
M. Pérez-Luna A. Cosultchi J. A. Toledo-Antonio C. Angeles-Chavez E. M. Arce-Estrada 《Catalysis Letters》2006,107(1-2):103-110
Three Ni/ZrO2–SO4=/Al2O3 catalysts with different concentrations of platinum (0.2, 0.3 and 0.4 wt%) were prepare and tested for n-butane isomerization reaction at 338 K, in absence and in presence of hydrogen. The results shown that, at low temperature,
platinum contributes to the olefin or butyl ion formation and the reaction follows a bimolecular pathway. However, when the
reaction occurs in the presence of hydrogen, the formation of butyl ions is inhibited. The main feature of platinum addition
is the stabilization of the catalytic activity, which is indicated by the slow deactivation constants compared to that of
the unpromoted catalyst. 相似文献
77.
The oxidation of acetaldehyde on carbon supported Pt/Vulcan, PtRu/Vulcan and Pt3Sn/Vulcan nanoparticle catalysts and, for comparison, on polycrystalline Pt and on an unsupported PtRu0.2 catalyst, was investigated under continuous reaction and continuous electrolyte flow conditions, employing electrochemical and quantitative differential electrochemical mass spectroscopy (DEMS) measurements. Product distribution and the effects of reaction potential and reactant concentration were investigated by potentiodynamic and potentiostatic measurements. Reaction transients, following both the Faradaic current as well as the CO2 related mass spectrometric intensity, revealed a very small current efficiency for CO2 formation of a few percent for 0.1 m acetaldehyde bulk oxidation under steady-state conditions on all three catalysts, the dominant oxidation product being acetic acid. Pt alloy catalysts showed a higher activity than Pt/Vulcan at lower potential (0.51 V), but do not lead to a better selectivity for complete oxidation to CO2. C–C bond breaking is rate limiting for complete oxidation at potentials with significant oxidation rates for all three catalysts. The data agree with a parallel pathway reaction mechanism, with formation and subsequent oxidation of COad and CH
x, ad species in the one pathway and partial oxidation to acetic acid in the other pathway, with the latter pathway being, by far, dominant under present reaction conditions. 相似文献
78.
超细镍基负载型催化剂成型工艺条件研究 总被引:3,自引:2,他引:3
以正硅酸乙酯、钛酸丁酯、硝酸镍为主要原料,采用溶胶-凝胶法(Sol-gel)实验室放大制备10 kg工业中试用催化剂粉料,加胶粘剂A进行挤条成型。催化剂前躯体的物化性能用BET、XRD、TG-DTA、TEM及强度测试仪进行表征,用固定床连续流动微反装置,考察催化剂苯加氢生成环己烷的催化性能。研究结果表明,催化剂的强度随胶粘剂的含量增大而增大,当胶粘剂含量达到13%时,NiO/SiO2-TiO2体系产生了新的晶相。胶粘剂的含量对催化剂的催化性能影响很小,该催化剂应用于苯加氢制环己烷实验中,苯转化率均为100%,环己烷的选择性均达到99.0%以上。 相似文献
79.
Pt/Al2O3 catalysts with platinum contents of 0.1, 1.0 and 3.0 wt% were used for the low temperature combustion of methanol in the absence and the respective presence of a trace amount of ammonia. It is observed that ammonia inhibits the combustion of methanol, which is due to competition between methanol and ammonia for the same sites. For a fixed space velocity and without ammonia in the gas, the performances of the catalysts increase up to a Pt loading of 1.0 wt%. In the presence of ammonia, however, no upper limit of performance is observed with increased Pt content. The results are discussed in terms of both Pt–support interface and the Pt surface being active. 相似文献
80.
In this work, ethylene was polymerized by using Cp2ZrCl2 supported on silica pretreated with methylaluminoxane (MAO) as the catalyst system. The influence of the conditions for the preparation of the heterogeneous catalyst, such as temperature, washing method of the catalytic solid, MAO and metallocene concentration in the support treatment, time of MAO, and metallocene immobilization on the support, type of alkylaluminum used in the support pretreatment, and calcination temperature of the support were investigated. Aluminum and zirconium content fixed on the silica surface were determined by inductively coupled plasma emission spectroscopy. Polymer characteristics were determined by gel permeation chromatography and differential scanning calorimetry. According to the results, the activity of some supported catalysts were far higher than with the homogeneous system. Moreover, polyethylene with very high molecular weights were also obtained and with molecular weight distribution larger than those produced with the homogeneous precursor. © 2002 Wiley Periodicals, Inc. J Appl Polym Sci 86: 2054–2061, 2002 相似文献