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101.
CeO2–ZrO2–La2O3 (CZL) mixed oxides were prepared by citric acid sol–gel method. The as-received gel was calcined at 500, 700, 900 and 1050 °C to obtain the so-called C5, C7, C9 and CK, respectively. The C5, C7 and C9 powders were impregnated with H2PtCl6 and then calcined at 500 °C to prepare P5C5, P5C7 and P5C9, respectively. The impregnated CK powders were calcined at 500, 700 and 900 °C to prepare P5CK, P7CK and P9CK, respectively. The XRD and XPS analyses show that the surface distribution of Pt is evidently influenced by the structural and textural properties of the support. The CO adsorption followed by FTIR reveals that the dispersion and the chemisorption sites of Pt are reduced as the calcination temperature of CZL support increases. The chemisorption ability of the CK samples is even completely deactivated. The encapsulation mechanism, which has been applied to explain the so-called strong metal–support interaction (SMSI) after reductive treatment, is introduced here to demonstrate the abnormal observations though the samples were prepared in oxidative atmosphere. The HRTEM results also confirm this explanation. The effects of oxygen vacancies, the chemisorption sites on the Pt surface and Pt/Ce interfacial sites on the three-way catalytic activities are discussed. 相似文献
102.
Shigeru Sugiyama Kiyozumi Sato Seiji Yamasaki Katsuhiro Kawashiro Hiromu Hayashi 《Catalysis Letters》1992,14(1):127-133
Silica-supported alkaline earth oxides revealed excellent activity to convert acetic acid selectively into acetone in a vapor-phase fixed-bed flow system. Acetone was obtained through the cyclic formation of alkaline earth acetate followed by decomposition. Magnesium oxide should be supported on the silica surface without formation of magnesium silicate, which was inactive for the present reaction. Attempted syntheses of benzophenone and acetophenone are also described. 相似文献
103.
Alumina supported vanadia catalysts (V/Al) for selective oxidehydrogenation of ethylbenzene with CO2 were prepared by impregnation method. During preparation the effect of promoters and calcined temperature was investigated,
it was found these two items had a strong influence on the activity of V/Al catalysts. Dehydrogenation reaction with CO2 was happened in the fixed-bed reactor at 450 °C. Results showed that 15.2% ethylbenzene conversion and 99.2% styrene selectivity
were acquired when V2K/Al catalyst was used. 相似文献
104.
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
105.
二氧化钛固载杂多酸催化剂的制备及其光催化性能研究 总被引:7,自引:2,他引:7
采用浸渍法以TiO2为载体制备了固载型杂多酸光催化剂--H3PW12O40/TiO2,H8SiW12O42/TiO2,H7PMo12O42/TiO2.通过Hammett指示剂与紫外光谱相结合的方法测定固体杂多酸催化剂的酸度,分别考察杂多酸种类、浸渍时间、浸渍浓度、烧结方式、烧结温度对催化剂酸度的影响,并对所制备的催化剂进行了红外光谱和光催化活性测试.结果表明,杂多酸固载到TiO2的表面,得到了催化活性较TiO2更强的复合杂多酸光催化剂,其对酸性大红3R的降解率从纯TiO2的79%提高到91%.以磷钨酸水溶液浸渍TiO2,浸渍浓度为0.10 mol·L-1 ,浸渍时间为28 h,烘干温度为120℃,微波炉焙烧功率为650 W,烧结时间为40 min制得的催化剂活性最高.在HPA-TiO2光催化系统中,杂多酸显著加速电子从TiO2表面到O2分子的传递,改变了TiO2光催化反应历程,从而提高光催化效率. 相似文献
106.
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
107.
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
108.
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
109.
110.
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