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1.
In this study, the decomposition of methanol into the CO and H species on the Pd/tungsten carbide (WC)(0001) surface is systematically investigated using periodic density functional theory (DFT) calculations. The possible reaction pathways and intermediates are determined. The results reveal that saturated molecules, i.e., methanol and formaldehyde, adsorb weakly on the Pd/ WC(0001) surface. Both CO and H prefer three-fold sites, with adsorption energies of −1.51 and −2.67 eV, respectively. On the other hand, CH3O stably binds at three-fold and bridge sites, with an adsorption energy of −2.58 eV. However, most of the other intermediates tend to adsorb to the surface with the carbon and oxygen atoms in their sp3 and hydroxyl-like configurations, respectively. Hence, the C atom of CH2OH preferentially attaches to the top sites, CHOH and CH2O adsorb at the bridge sites, while COH and CHO occupy the three-fold sites. The DFT calculations indicate that the rupture of the initial C–H bond promotes the decomposition of CH3OH and CH2OH, whereas in the case of CHOH, O–H bond scission is favored over the C–H bond rupture. Thus, the most probable methanol decomposition pathway on the Pd/WC(0001) surface is CH3OH → CH2OH → trans-CHOH → CHO → CO. The present study demonstrates that the synergistic effect of WC (as carrier) and Pd (as catalyst) alters the CH3OH decomposition pathway and reduces the noble metal utilization. 相似文献
2.
A self-assembled monolayer (SAM) of p-hydroxymethylbenzene HOCH2C6H4 - (HOMB) moiety adsorbed on iron by the formation of a covalent bond between carbon and iron atoms was prepared by electrochemical derivatization of an iron electrode with p-hydroxymethylbenzenediazonium tetrafluoroborate HOCH2C6H4N2BF4. The electrode covered with the HOMB SAM was modified with alkyltriethoxysilanes CnH2n+1Si(OC2H5)3 (CnTES, n = 8 or 18) to prepare a film of one-dimensional polymer. The protective ability of the polymer film was determined by polarization measurement of the covered electrode in an aerated 0.5 M NaCl solution. The ability was enhanced by modification of the HOMB SAM with CnTES markedly. The iron surface coated with the one-dimensional polymer film of the HOMB SAM modified with C8TES was characterized by contact angle measurement and FTIR reflection and X-ray photoelectron spectroscopies. The persistence in the protective ability of the polymer film against iron corrosion in 0.5 M NaCl may be associated with the strong adsorption via the covalent bond, revealed by electron-probe microanalysis. 相似文献
3.
4.
R. Meyer Hilde Hardtdegen R. Carius D. Grützmacher M. Stollenwerk P. Balk A. Kux B. Meyer 《Journal of Electronic Materials》1992,21(3):293-298
This paper presents a study of the structural and optical properties of strained GaInAs/ InP multiple quantum well (MQW) structures
fabricated by LP-MOVPE. The composition of the Ga
x
In1−x
As films ranged fromx = 0.17 tox = 1.0 and was determined by sputtered neutral mass spectrometry (SNMS) on thick layers. The structures of the MQW samples
with well widths from 1.5 to 5 nm were investigated by high resolution x-ray diffraction (HR-XRD). Simulations of the diffraction
patterns showed that transition layers of approximately 2 monolayer (ML) thickness with high lattice mismatch exist at the
interfaces. Photoluminescence (PL) measurements indicate well widths of a multiple of a monolayer with local variations of
one monolayer. The PL peak energies vary smoothly with the Ga concentration. These results were confirmed by optical absorption
measurements. 相似文献
5.
Vibrational mode in a two-dimensional dust monolayer is investigated by considering the finite size of dust grains. Each dust grain is assumed to be a negative point charge and a dipole moment due to the inhomogeneous charge distribution on its surface. The dispersion relation of the vibrational mode is derived. Both the self-excited and externally excited cases are discussed. It is shown that the mode is sensitive to the direction of the dipole moment. 相似文献
6.
Upon the application of amperometric biosensor to the biological fluid, ascorbic acid interferes the amperometric determination of analytes, because the oxidative potential of ascorbic acid is lower than that of electro active substances such as H2O2 produced by the enzymatic reaction. In this study we propose a method to block ascorbic acid based on the electrostatic interaction with self-assembled monolayer (SAM) and its application of the surface modified electrode to biosensor. In order to form SAM on the gold electrode with carboxyl group, 7-carboxy-heptanethiol (7-CHT) was used. The 7-CHT modified electrode did not show anodic response to ascorbic acid, but oxidized phenanthroline cobalt complex [Co(phen)32+], which can be used as a mediator of biosensor. Thus, the 7CHT-modified electrode was applied to biosensor mediated with Co(phen)32+. Fructose dehydrogenase (FDH) was immobilized to the 7-CHT modified electrode. Fructose was determined selectively with the FDH/7-CHT modified electrode at the range of 0.2-2 mM. 相似文献
7.
L. A. Gioielli R. N. M. Pitombo M. Vitolo R. Baruffaldi M. N. Oliveira M. S. Augusto 《Journal of the American Oil Chemists' Society》1994,71(6):579-582
The lipase-catalyzed interesterification of oils and fats gives products that are unobtainable by chemical interesterification
methods. Acidolysis of babassu fat and palmitic acid, catalyzed by immobilized lipase (Lipozyme; Novo Industri, Bagsveard,
Denmark), was studied. The reactions were performed at 65°C with 5% w/w enzyme for 4 h. The molar proportions of babassu fat/palmitic
acid were 1∶0.1, 1∶0.3 and 1∶0.5. At the end of the reaction period, the catalyst particles were removed by filtration, and
the residual oil was extracted with organic solvent (diethyl ether). The recovered particles were then reused. The palmitic
acid content of babassu fat before and after acidolysis changed from 10 to 22% at a molar proportion of 1∶0.5. The equilibrium
was attained in about 4 h. The original water and enzymatic activities of Lipozyme were maintained after acidolysis. Water
sorption isotherms of the immobilized enzyme were determined at 25, 35 and 45°C. From the temperature dependence of the isotherms,
isosteric heats of sorption were evaluated by means of the Clausius Clapeyron equation. Monolayer moisture content was calculated
by means of the B.E.T. and Guggenhein-Anderson-De Boer analyses.
Paper presented at the International Meeting on Fats and Oils Technology, Universidade Estadual de Campinas, Brazil, 1991. 相似文献
8.
摘要:细胞固定化技术具有流程简单、生物相容、操作稳定等优点,可有效保证细胞活性,实现高效的细胞催化生产精细化学品。本文介绍了表面附着、凝胶包埋、聚电解质层层自组装膜等多细胞固定化方法,及其在二元醇、生物乙醇、乳酸、酯、多糖等精细化学品生产中的研究现状和进展,并分析讨论了各种方法存在的问题。同时,总结了近年来新发展的单细胞纳米涂层固定化方法的机理、趋势及应用于精细化学品生产的可能性。最后对细胞固定化催化生产精细化学品面临的技术挑战及研究方向做出展望,以期为精细化学品生产提供一定的技术支持。 相似文献
9.
Yuko Habuta Naoaki Narishige Kazu Okumura Naonobu Katada Miki Niwa 《Catalysis Today》2003,78(1-4):131-138
Vanadium oxide spread highly on TiO2 (anatase, A) and SnO2, and rather densely on TiO2 (rutile, R) and ZrO2 to make the monolayer in less than 4–5 V nm−2. Profile of acid site of the monolayer was measured by temperature programmed desorption of ammonia, and its relation with the surface oxidation state was studied. The acid site density was high on the V2O5/TiO2 (A) independent of the degree of oxidation. On the other hand, that of V2O5/TiO2 (R) and V2O5/ZrO2 depended on the oxidation state, and the high value of the concentration was observed on the oxidized one. The strength of acid site generated on the V2O5 monolayer on TiO2 was as high as on the HZSM-5 zeolite. Turnover frequency (TOF) of propane conversion, and product selectivity were measured in propane oxidation. Among tested oxides, the V2O5/TiO2 (A) showed the high TOF and selectivity to form propylene, while those loaded on TiO2 (R) and ZrO2 the small TOF and poor selectivity. Therefore, the reaction profile of activity and selectivity could be related with the extent of spreading and solid acidity. An idea of limit of the acid site density ca. 1.5 nm−2 on the monolayer was elucidated. 相似文献
10.