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71.
对无氧条件下Pt/TiO_2光催化重整甲醇制氢的基本步骤进行简化,在同一体系中进行了光催化剂的合成和光催化制氢的两步反应。基于正交设计法对该复杂体系进行了分析,得到Pt载量、甲醇/水体积、灯距、前反应时间这4种影响因素的3个不同水平对放氢速率的影响。确定了最佳实验条件为Pt载量0.5%(mol)、甲醇/水体积比5:1、灯距12 cm、前反应时间3h。分析结果表明,Pt载量对放氢速率的影响最大。实验获得的最高放氢速率为5.84 ml·h~(-1)·g~(-1)。 相似文献
72.
Eun-Yong Ko Eun Duck Park Kyung Won Seo Hyun Chul Lee Doohwan Lee Soonho Kim 《Korean Journal of Chemical Engineering》2006,23(2):182-187
Selective CO oxidation in the presence of excess hydrogen was studied over supported Pt catalysts promoted with various transition
metal compounds such as Cr, Mn, Fe, Co, Ni, Cu, Zn, and Zr. CO chemisorption, XRD, TPR, and TPO were conducted to characterize
active catalysts. Among them, Pt-Ni/γ-Al2O3 showed high CO conversions over wide reaction temperatures. For supported Pt-Ni catalysts, Alumina was superior to TiO2 and ZrO2 as a support. The catalytic activity at low temperatures increased with increasing the molar ratio of Ni/Pt. This accompanied
the TPR peak shift to lower temperatures. The optimum molar ratio between Ni and Pt was determined to be 5. This Pt-Ni/γ A12O3 showed no decrease in CO conversion and CO2 selectivity for the selective CO oxidation in the presence of 2 vol% H2O and 20 vol% CO2. The bimetallic phase of Pt-Ni seems to give rise to stable activity with high CO2 selectivity in selective oxidation of CO in H2-rich stream. 相似文献
73.
Preparation of anodes for oxygen evolution in seawater electrolysis was carried out. Manganese-molybdenum double oxides, Mn1−xMoxO2+x, prepared by anodic deposition from MnSO4-Na2MoO4 solutions showed the 100% oxygen evolution efficiency at a current density of 1000 A m−2 in 0.5 M NaCl at 30 °C and pH 12, but an increase in solution temperature resulted in dissolution of the oxides as molybdate and permanganate ions. In order to increase the stability of the electrodes at higher temperatures the addition of iron to the manganese-molybdenum oxides was performed by anodic deposition in MnSO4-Na2MoO4-FeNH4(SO4)2 solutions. The electrodes thus prepared showed the 100% oxygen evolution efficiency at 1000 A m−2 in 0.5 M NaCl at 30-90 °C, when proper amounts of molybdenum and iron were contained. The iron addition also enhanced the oxygen evolution efficiency. The electrodes were not composed of oxide mixtures but triple oxides, Mn1−x−yMoxFeyO2+x−0.5y, consisting of Mn4+, Mo6+ and Fe3+. The formation of the triple oxides seemed responsible for enhancement of both oxygen evolution efficiency and stability. 相似文献
74.
Evgeny Shustorovich 《Catalysis Letters》1990,7(1-4):107-118
We have applied the BOC-MP method to theoretically analyze the metal effects in the Fischer-Tropsch (FT) synthesis by calculating the energetics of conceivable elementary steps (the relevant heats of chemisorption and the reaction activation barriers) during CO hydrogenation over the periodic series Fe(110), Ni(111), Pt(111), Cu(111). The basic steps such as dissociation of CO, hydrogenation of carbidic carbon, C-C chain growth by insertion of CH2 versus CO into the metal-alkyl bonds, and chain termination leading to hydrocarbons (alkanes versus -olefins) or oxygenates are discussed in detail. It is shown that the periodic trends in the ability of metal surfaces to dissociate chemical bonds and those to recombine the bonds are always opposite. In particular, we argue that metallic Fe is necessary to produce the abundance of carbidic carbon from CO but the synthesis of hydrocarbons and oxygenates can effectively proceed only on carbided Fe surfaces which resemble the less active metals such as Pt. More specifically, we project that the C-C chain growth should occur predominantly via CH2 insertion into the metal-alkyl bond and the primary FT products should be -olefins. These and other model projections are in agreement with experiment. 相似文献
75.
Ralf Dümpelmann Noel W. Cant David L. Trimm 《Applied catalysis. B, Environmental》1995,6(4):L291-L296
On-line infrared spectroscopy has been used to show that isocyanic acid, HNCO, is a substantial primary product of the reaction between NO, CO and H2 over a Pt/SiO2 catalyst. At 230°C it accounts for more than 40% of the CO converted. No isocyanic acid is seen when Al2O3 is placed downstream of Pt/SiO2, or when using a Pt/Al2O3 catalyst under the same conditions, due to rapid hydrolysis of HNCO on the alumina. Isocyanic acid may exist as a trace intermediate in automobile catalytic converters during their warm-up phase but it is unlikely to emerge from the pore system of aluminabased catalysts. 相似文献
76.
The oxidation and reforming kinetics of methane by O2, CO2 and H2O were studied on a stepped Pt(5 5 7) single crystal from 623 to 1050 K under methane rich conditions. The rate of carbon deposition was followed by ex-situ Auger electron spectroscopy under non-oxidative conditions. The apparent activation energy for methane decomposition was significantly lower than the apparent barriers measured for both total oxidation, CO2 and H2O reforming. Total oxidation of methane to CO2 and H2O followed by combined dry and steam reforming (combined combustion-reforming) led to CO production rates which were higher than direct CO2 or H2O reforming rates. The enhanced rates are most likely due to the ability of adsorbed oxygen to prevent carbon nucleation and/or scavenge carbon enabling the reforming reaction to turnover on a larger fraction of sites. Comparable amounts of carbon were found by Auger electron spectroscopy measurements after both direct dry or steam reforming, while combined oxidation-reforming had considerable less carbon. During direct dry or steam reforming, CO2 and H2O serve only to scavenge adsorbed atomic carbon, while in the presence of oxygen, carbon is removed by both combustion and reforming routes. 相似文献
77.
CeO2 particles confined within the pores of an SBA-15 mesoporous silica host were prepared by incipient wetness impregnation (IMP)
and deposition precipitation (DP) methods. The materials were characterized by XRD, N2-adsorption and temperature programmed reduction (TPR) to evaluate the structure, texture, and redox properties. The preparation
procedure had significant impact on the assembling mode of CeO2 inside the SBA-15 mesopores. A high dispersion of CeO2 particles was achieved via DP, whereas the dispersion of CeO2 prepared by IMP was found to be inhomogeneous and CeO2 partially blocked the pores. The CO conversion in the water-gas-shift reaction was enhanced over 1 wt% Pt supported on CeO2-modified SBA-15 obtained by DP. 相似文献
78.
Novel NOx storage-reduction (NOxSR) catalysts prepared by Pt and/or Cu impregnation of Mg–Al (60:40) hydrotalcite (HT)-type compounds show better performances in NOx storage than Pt–Ba/Al2O3 Toyota-type NOxSR catalysts at reaction temperatures lower than 250 °C. The presence of Pt or Cu considerably enhances the activity, with the former more active. The nature of the HT source, however, also influences performance. The co-presence of Pt and Cu slightly worsens the low temperature activity, but considerably promotes the resistance to deactivation after severe hydrothermal treatment and in the presence of SO2. This effect is attributed to both the possibility of formation of a Pt–Cu alloy after reduction, and the modification of the HT induced during the deposition of Cu. The overall Pt–Cu/HT performances are thus superior to those of the Pt–Ba/Al2O3 Toyota-type NOxSR catalysts. 相似文献
79.
An effect of oxygen species formed from O2, N2O and NO on the selectivity of the catalytic oxidation of ammonia was studied over a polycrystalline Pt catalyst using the temporal analysis of products (TAP) reactor. The transient experiments were performed in the temperature range between 773 and 1073 K in a sequential pulse mode with a time interval of 0.2 s between the pulses of the oxidant (O2, N2O and NO) and NH3. In contrast to adsorbed oxygen species formed from NO, those from O2 and N2O reacted with ammonia yielding NO. It is suggested that the difference between these oxidising agents may be related to the different active sites for dissociation of O2, N2O and NO, where oxygen species of various Pt-O strength are formed. Weaker bound oxygen species, which are active for NO formation, originate from O2 and N2O rather than from NO. These species may be of bi-atomic nature. 相似文献
80.
非离子胶束对竹红菌乙素及其溴代物基态和激发态的保护作用 总被引:8,自引:0,他引:8
本文用Triton-X-100非离子型胶束增溶生红菌乙素及其两种溴代物,发现该胶束对HB的基态和激发态都有保护作用;(1)HB基态的ρKa升高;(2)荧光量子产率增大。这使其光敏反应产生的活性中间体^1O2和.OH的产额增加,从而增强了其光敏活性。 相似文献