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101.
T.V. Choudhary A.K. Santra C. Sivadinarayana B.K. Min C.-W. Yi K. Davis D.W. Goodman 《Catalysis Letters》2001,77(1-3):1-5
Ammonia decomposition on Ir(100) has been studied over the pressure range from ultrahigh vacuum to 1.5 Torr and at temperatures ranging from 200 to 800 K. The kinetics of the ammonia decomposition reaction was monitored by total pressure change. The apparent activation energy obtained in this study (84 kJ/mol) is in excellent agreement with our previous studies using supported Ir catalysts (Ir/Al2O3 82 kJ/mol). Partial pressure dependence studies of the reaction rate yielded a positive order (0.9±0.1) with respect to ammonia and negative order (–0.7 ±0.1) with respect to hydrogen. Temperature-programmed desorption data from clean and hydrogen co-adsorbed Ir(100) surfaces indicate that ammonia undergoes facile decomposition on both these surfaces. Recombinative desorption of N2 is the rate-determining step with a desorption activation energy of 63 kJ/mol. Co-adsorption data also indicate that the observed negative order with respect to hydrogen pressure is due to enhancement of the reverse reaction (NH
x
+ H NH
x+1, x=0–2) in the presence of excess H atoms on the surface. 相似文献
102.
The equilibrium phase compositions of iron have been calculated for gas compositions that could be encountered during the Fischer–Tropsch synthesis. The gas compositions measured experimentally for CO conversion levels in the 30–90% range show that iron should be present as the carbide phase. However, experimental characterization of iron catalysts show that a significant fraction of the iron is present as Fe3O4 following synthesis for several days. A model that can account for the experimental catalyst phase composition and the gases present in the reactor would have a core of Fe3O4 and an outer layer of iron carbides. 相似文献
103.
A series of high performance, experimental carbon/graphite fibers was intercalated and examined with respect to their metallic conductivity behavior by resistivity and magnetoresistance versus temperature measurements. One fiber was a polyacrylonitrile (PAN)-type precursor and three were pitch base precursors. All four types showed substantially similar behavior in the pristine state with respect to room temperature resistivity and the sign and magnitude of the temperature coefficient of resistivity. After intercalation with either nitric acid or nitric acid followed by AsF5, the PAN-based fibers displayed a resistivity versus temperature behavior qualitatively similar to their pristine counterparts but displaced to lower resistivity. On the other hand, the pitch fibers with the same intercalation treatment exhibited metallic behavior (a positive temperature coefficient of electrical resistivity and a small magnetoresistance). These manifestations of metallic behavior are usually indicative of some three dimensional graphite structure in the carbon fibers. 相似文献
104.
Gold particles supported on carbon and titania were explored as catalysts for oxidation of CO or glycerol by O2 at room temperature in liquid-phase water. Although Au/carbon catalysts were not active for vapor phase CO oxidation at room
temperature, a turnover frequency of 5 s−1 could be achieved with comparable CO concentration in aqueous solution containing 1 M NaOH. The turnover frequency on Au/carbon
was a strong function of pH, decreasing by about a factor of 50 when the pH decreased from 14 to 0.3. Evidently, a catalytic
oxidation route that was not available in the vapor phase is enabled by operation in the liquid water at high pH. Since Au/titania
is active for vapor phase CO oxidation, the role of water, and therefore hydroxyl concentration, is not as significant as
that for Au/carbon. Hydrogen peroxide is also produced during CO oxidation over Au in liquid water and increasing the hydroxyl
concentration enhances its formation rate. For glycerol oxidation to glyceric acid (C3) and glycolic acid (C2) with O2 (1–10 atm) at 308–333 K over supported Au particles, high pH is required for catalysis to occur. Similar to CO oxidation
in liquid water, H2O2 is also produced during glycerol oxidation at high pH. The formation of the C-C cleavage product glycolic acid is attributed
to peroxide in the reaction. 相似文献
105.
A theory of the wetting of solids by liquids is put forward. The theory accounts for capillary pressure gradient, gravitational potential gradient, surface tension gradient, disjoining pressure gradient driving forces of flow in thick thin-films and of surface diffusion in thin thin-films. Disjoining pressure stems from the way intermolecular forces aggregate in submicroscopically thin films. For thick thin-films of slowly varying thickness the lubrication approximation to velocity distributions is appropriate. With this approximation the spontaneous, unsteady, two-dimensional spreading of liquid is shown to be governed by a nonlinear convective-diffusion equation for the evolution of the film thickness profile. The predictions of the theory agree with Marmur and Lelah's (1980, 1981) observations of water drops spreading on glass and with Bascom, Cottington and Singleterry's (1964) and Ludviksson and Lightfoot's (1971) observations of oils spreading on high energy surfaces. The theory is used to analyze Derjaguin and co-workers' (1944, 1957, 1970) blowing-off experiments designed to measure thin-film rheology. The theory is also used to buttress the proposition that much contact angle hysteresis is due simply to slow attainment of equilibrium. 相似文献
106.
Kuo-Hao Lee Yongjian Yang Linfeng Ding Benedikt Ziebarth Mark J. Davis John C. Mauro 《Journal of the American Ceramic Society》2021,104(7):3073-3086
The shear behaviors of two multicomponent borosilicate glasses, Borofloat®33 (Boro33) and N-BK7® (N-BK7), under different pressures are investigated using molecular dynamics simulations. The addition of alkali ions lowers the yield stress and changes the pressure dependence of shear modulus. Shear-induced densification is observed in both glasses. It is found that the decreases of the oxygen-centered bond angle and the coordination number change of B are responsible for the density changes at low pressures, and the increase of 5-coordinated Si is the dominant mechanism for densification at high pressures. The average shear stresses experienced by Si and B decrease with pressure except that the flow stress of Si at the end of shear deformation in N-BK7. Moreover, the average shear stress of B is more sensitive to the applied pressures compared to Si, suggesting that B is able to relax mechanical stress more easily under pressurized-shear. By analyzing the nonaffine displacement of atoms, it is found that N-BK7 exhibits more localized plastic deformation compared to Boro33 at low pressures and the local rearrangements in both glasses become more homogeneous with increasing pressure. The mean squared nonaffine displacement curves show that alkali ions have the highest mobility induced by shear compared to the network formers and B is more mobile than Si for both glasses. We also observed that plastic deformation tends to take place around boron atoms for Boro33, whereas it occurs in the alkali-rich regions for N-BK7, indicating that these two glasses have different atomic-scale deformation mechanisms. 相似文献
107.
Kuo-Hao Lee Yongjian Yang Linfeng Ding Benedikt Ziebarth Mark J. Davis John C. Mauro 《Journal of the American Ceramic Society》2021,104(6):2506-2520
Knowledge of the underlying structural response during deformation processes is essential for understanding the macroscopic mechanical response of glass. Here we present results from cold compression-decompression molecular dynamics (MD) simulations of two multicomponent borosilicate glasses, Borofloat®33 (Boro33) and N-BK7® (N-BK7). Our results suggest that the densification of these two borosilicate glasses involves different types of structural changes. The fraction of permanent densification can be correlated to the change in intermediate-range structure. By performing Voronoi analysis, we quantify the contributions to densification from different cation types in these two multicomponent borosilicate glasses, finding that 3-coordinated cations facilitate the densification process. Higher-coordinated cations are relatively stable and can even show a slight expansion in their Voronoi volume. 相似文献
108.
109.
Richard O. Sinnott Christopher Bayliss Andrew Bromage Gerson Galang Yikai Gong Philip Greenwood Glenn Jayaputera Davis Marques Luca Morandini Ghazal Nogoorani Hossein Pursultani Muhammad Sarwar William Voorsluys Ivo Widjaja 《Journal of Grid Computing》2016,14(4):603-618
Big data technologies and a range of Government open data initiatives provide the basis for discovering new insights into cities; how they are planned, how they managed and the day-to-day challenges they face in health, transport and changing population profiles. The Australian Urban Research Infrastructure Network (AURIN – www.aurin.org.au) project is one example of such a big data initiative that is currently running across Australia. AURIN provides a single gateway providing online (live) programmatic access to over 2000 data sets from over 70 major and typically definitive data-driven organizations across federal and State government, across industry and across academia. However whilst open (public) data is useful to bring data-driven intelligence to cities, more often than not, it is the data that is not-publicly accessible that is essential to understand city challenges and needs. Such sensitive (unit-level) data has unique requirements on access and usage to meet the privacy and confidentiality demands of the associated organizations. In this paper we highlight a novel geo-privacy supporting solution implemented as part of the AURIN project that provides seamless and secure access to individual (unit-level) data from the Department of Health in Victoria. We illustrate this solution across a range of typical city challenges in localized contexts around Melbourne. We show how unit level data can be combined with other data in a privacy-protecting manner. Unlike other secure data access and usage solutions that have been developed/deployed, the AURIN solution allows any researcher to access and use the data in a manner that meets all of the associated privacy and confidentiality concerns, without obliging them to obtain ethical approval or any other hurdles that are normally put in place on access to and use of sensitive data. This provides a paradigm shift in secure access to sensitive data with geospatial content. 相似文献
110.
Varol O. Kayhan Christopher J. Davis Rosann Webb Collins Anol Bhattacherjee 《Information Systems Management》2013,30(2):168-178
Two mechanisms that verify knowledge contributions in electronic repositories are expert-governance and community-governance. Our goal is to examine repository users' perceptions of the conditions under which these mechanisms verify knowledge contributions. Qualitative data show that perceived credibility of experts, perceived ownership of content, and experts' (meticulous) execution of governance functions are salient for expert-governance, and the perceived involvement of community members, and community members' (continuous and collective) execution of governance functions are important for community-governance. 相似文献