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71.
72.
Ana Lúcia Cardoso Manuela Ramos Silva Francisco Palacios Alberto A.C.C. Pais 《Tetrahedron》2010,66(39):7720-7725
Stereoselective inverse conjugate addition of carbonucleophiles to allenoates bearing a chiral auxiliary in the ester moiety afforded optically active α,β-unsaturated carboxylic esters bearing a new stereocenter at the δ position. The rationalization of the observed selectivity was supported by semi-empirical molecular orbital calculations. 相似文献
73.
The synthesis of a stable ketene aminal phosphate (α-phosphoryloxy enecarbamate) derived from N,N-diprotected acetamide, bearing two different removable protecting groups, is disclosed. This synthetic intermediate underwent successful palladium-catalyzed cross-coupling reactions to afford functionalized enynes and dienes. 相似文献
74.
75.
采用三种不同方法制备了Cu-Zn-Al基甲醇催化剂,然后在水相悬浮液中与H型镁碱沸石混合分散,以制得负载型甲醇催化剂.运用X射线衍射、N2吸附-脱附、透射电镜、程序升温还原、NH3程序升温脱附、H2程序升温脱附和X射线光电子能谱对催化剂进行了表征.考察了催化剂催化CO加氢反应生成二甲醚和烃类的性能.该催化剂是在低和高过饱和度条件下采用共沉淀法和均匀沉淀法制得的.制备方法对前驱体的结构特性(如纯度、结晶度和催化剂颗粒粒径分布)有显著影响.低过饱和度的沉淀条件有利于Cu物种的高度分散,增加了催化剂中金属的比表面积,所得催化剂粒径分布均匀.这些效应进而会影响分子筛的性质,导致其微孔孔体积较小,分子筛酸性位被堵塞.通过Cu比表面积和CO转化速率之间的关联可考察甲醇催化剂的性能. 相似文献
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77.
Cesar M. C. Filho Manoel N. L. Neto Raquel S. Teixeira Alberto A. C. C. Pais 《液相色谱法及相关技术杂志》2016,39(19-20):837-846
Benzene, toluene, and xylene isomers (BTXs) and pyrene, benzo(b)fluoranthene, and benzo(a)pyrene (polycyclic aromatic hydrocarbons) are common pollutants found in many industrial effluents and in aquifers due to fossil fuels spill from underground storage reservoirs. For these reasons, the determination of these compounds has gained importance in the last decades. In this work, a simultaneous, fast, and accurate quantification of six petroleum hydrocarbon compounds (such as BTXs, pyrene, benzo(b)fluoranthene, and benzo(a)pyrene) using a high-performance liquid chromatography–diode array detector method has been demonstrated. The proposed method is suitable for the direct aqueous sample evaluation and also brings advantages, including the use of small volumes of organic solvents, with high resolution, reducing the analysis cost. The method was also checked using synthetic and real samples, including those containing surfactants, commercial gasoline, and river water samples spiked with petroleum hydrocarbon compounds. 相似文献
78.
The distribution of neutral and charged polymers with different flexibilities between two spheres of varying volume connected by a short and narrow cylinder has been investigated by Monte Carlo simulations. The uncharged chain displayed mostly a single-sphere occupancy due to the high conformational entropy penalty of crossing the cylindrical domain, whereas for the charged polymer a double-sphere occupancy was obtained, except for very different spherical volumes. The origin of this different occupancy behavior stems from the counterion entropy. At increasing stiffness, a stronger preference for double-sphere occupancy was predicted. 相似文献
79.
Arnaut LG Pais AA Formosinho SJ Barroso M 《Journal of the American Chemical Society》2003,125(17):5236-5246
We calculate transition-state energies of atom-transfer reactions from reaction energies, electrophilicity indices, bond lengths, and vibration frequencies of the reactive bonds. Our calculations do not involve adjustable parameters and uncover new patterns of reactivity. The generality of our model is demonstrated comparing the vibrationally adiabatic barriers obtained for 100 hydrogen-atom transfers with the corresponding experimental activation energies, after correction for the heat capacities of reactants and transition state. The rates of half of these reactions are calculated using the Transition-State Theory with the vibrationally adiabatic path of the Intersecting-State Model and the semiclassical correction for tunneling (ISM/scTST). The calculated rates are within an order of magnitude of the experimental ones at room temperature. The temperature dependencies and kinetic isotope effects of selected systems are also in good agreement with the available experimental data. Our model elucidates the roles of the reaction energy, electrophilicity, structural parameters, and tunneling in the reactivity of these systems and can be applied to make quantitative predictions for new systems. 相似文献
80.