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991.
Thamina Akther Md.Monarul Islam Taisuke Matsumoto Junji Tanaka Pierre Thuéry Carl Redshaw Takehiko Yamato 《Tetrahedron》2018,74(2):329-335
The reductive coupling reaction of 1,4-bis(3-acetyl-5-tert-butyl-2-methoxyphenyl)butane 3 was carried out using TiCl4-Zn in pyridine followed by a McMurry coupling reaction to afford the compounds anti and syn 1,2-dimethyl[2.4]MCP-1-ene 4. Bromination of 4 with BTMA-Br3 in dry CH2Cl2 afforded the interesting compound 1,2-bis-(bromomethyl)-5,15-di-tert-butyl-8,18-dimethoxy[2.4]MCP-1-ene 6 and consecutive debromination with Zn and AcOH in CH2Cl2 solution afforded the stable solid 5,15-di-tert-butyl-8,18-dimethoxy-1,2-dimethylene[2.4]MCP 7 in 89% yield. Compound 7 was conveniently employed in a Diels–Alder reaction with dimethyl acetylenedicarboxylate (DMAD) to provide 2-(3′,6′-dihydrobenzo)-5,15-di-tert-butyl-8,18-dimethoxy[2.4]MCP-4′,5′-dimethylcarboxylate 8 in good yield. Diels–Alder adduct 8 was converted into a novel and inherently chiral areno-bridged compound [2.4]MCP 9 by aromatization. The chirality of the two conformers was characterized by circular dichroism (CD) spectra of the separated enantiomer which are perfect mirror images of each other. 相似文献
992.
Pierre Thuéry Martine Nierlich 《Journal of inclusion phenomena and macrocyclic chemistry》1997,27(1):13-20
The synthesis and crystal structure of the inclusion complex between uranyl and p-tert-butylcalix[5]arene are reported. [UO2 (p-tert-butylcalix[5]arene-4H]2- ·
&·2MeOH(1) crystallizes in the monoclinic space group C2/c, a = 30.06(2), b = 18.20(3), c = 31.35(2) Å, = 128.51(6)°, V = 13423(40) Å3, Z = 8. Refinement led to a final conventional R value of 0.043 for 4155 reflections. The uranyl ion is bonded, in its equatorial plane, to the five oxygen atoms of the calixarene, four of which are deprotonated. A protonated triethylamine molecule is located inside the calixarene cavity and hydrogen bonded to a uranyl oxygen atom, and another one outside and hydrogen bonded to a calixarene oxygen atom. The calixarene conformation is the usual cone one. 相似文献
993.
Alba Nicolas‐Boluda Zhijie Yang Illia Dobryden Florent Carn Naomi Winckelmans Christine Pchoux Pierre Bonville Sara Bals Per Martin Claesson Florence Gazeau Marie Paule Pileni 《Advanced functional materials》2020,30(40)
Control of interactions between nanomaterials and cells remains a biomedical challenge. A strategy is proposed to modulate the intralysosomal distribution of nanoparticles through the design of 3D suprastructures built by hydrophilic nanocrystals (NCs) coated with alkyl chains. The intracellular fate of two water‐dispersible architectures of self‐assembled hydrophobic magnetic NCs: hollow deformable shells (colloidosomes) or solid fcc particles (supraballs) is compared. These two self‐assemblies display increased cellular uptake by tumor cells compared to dispersions of the water‐soluble NC building blocks. Moreover, the self‐assembly structures increase the NCs density in lysosomes and close to the lysosome membrane. Importantly, the structural organization of NCs in colloidosomes and supraballs are maintained in lysosomes up to 8 days after internalization, whereas initially dispersed hydrophilic NCs are randomly aggregated. Supraballs and colloidosomes are differently sensed by cells due to their different architectures and mechanical properties. Flexible and soft colloidosomes deform and spread along the biological membranes. In contrast, the more rigid supraballs remain spherical. By subjecting the internalized suprastructures to a magnetic field, they both align and form long chains. Overall, it is highlighted that the mechanical and topological properties of the self‐assemblies direct their intracellular fate allowing the control intralysosomal density, ordering, and localization of NCs. 相似文献
994.
995.
Structure–Thermodynamic‐Property Relationships in Cyanovinyl‐Based Microporous Polymer Networks for the Future Design of Advanced Carbon Capture Materials 下载免费PDF全文
Ali Yassin Matthias Trunk Frank Czerny Pierre Fayon Abbie Trewin Johannes Schmidt Arne Thomas 《Advanced functional materials》2017,27(26)
Nitrogen‐rich solid absorbents, which have been immensely tested for carbon dioxide capture, seem until this date to be without decisive molecular engineering or design rules. Here, a family of cyanovinylene‐based microporous polymers synthesized under metal‐catalyzed conditions is reported as a promising candidate for advanced carbon capture materials. These networks reveal that isosteric heats of CO2 adsorption are directly proportional to the amount of their functional group. Motivated by this finding, polymers produced under base‐catalyzed conditions with tailored quantities of cyanovinyl content confirm the systematical tuning of their sorption enthalpies to reach 40 kJ mol?1. This value is among the highest reported to date in carbonaceous networks undergoing physisorption. A six‐point‐plot reveals that the structure–thermodynamic‐property relationship is linearly proportional and can thus be perfectly fitted to tailor‐made values prior to experimental measurements. Dynamic simulations show a bowl‐shaped region within which CO2 is able to sit and interact with its conjugated surrounding, while theoretical calculations confirm the increase of binding sites with the increase of Ph? C?C(CN)? Ph functionality in a network. This concept presents a distinct method for the future design of carbon dioxide capturing materials. 相似文献
996.
Sputtered Titanium Carbide Thick Film for High Areal Energy on Chip Carbon‐Based Micro‐Supercapacitors 下载免费PDF全文
Manon Létiche Kevin Brousse Arnaud Demortière Peihua Huang Barbara Daffos Sébastien Pinaud Marc Respaud Bruno Chaudret Pascal Roussel Lionel Buchaillot Pierre Louis Taberna Patrice Simon Christophe Lethien 《Advanced functional materials》2017,27(20)
The areal energy density of on‐chip micro‐supercapacitors should be improved in order to obtain autonomous smart miniaturized sensors. To reach this goal, high surface capacitance electrode (>100 mF cm?2) has to be produced while keeping low the footprint area. For carbide‐derived carbon (CDC) micro‐supercapacitors, the properties of the metal carbide precursor have to be fine‐tuned to fabricate thick electrodes. The ad‐atoms diffusion process and atomic peening effect occurring during the titanium carbide sputtering process are shown to be the key parameters to produce low stress, highly conductive, and thick TiC films. The sputtered TiC at 10?3 mbar exhibits a high stress level, limiting the thickness of the TiC‐CDC electrode to 1.5 µm with an areal capacitance that is less than 55 mF cm?2 in aqueous electrolyte. The pressure increase up to 10?2 mbar induces a clear reduction of the stress level while the layer thickness increases without any degradation of the TiC electronic conductivity. The volumetric capacitance of the TiC‐CDC electrodes is equal to 350 F cm?3 regardless of the level of pressure. High values of areal capacitance (>100 mF cm?2) are achieved, whereas the TiC layer is relatively thick, which paves the way toward high‐performance micro‐supercapacitors. 相似文献
997.
Layered Simple Hydroxides Functionalized by Fluorene‐Phosphonic Acids: Synthesis,Interface Theoretical Insights,and Magnetoelectric Effect 下载免费PDF全文
Quentin Evrard Ziyad Chaker Mélissa Roger Charlotte M. Sevrain Emilie Delahaye Mathieu Gallart Pierre Gilliot Cédric Leuvrey Jean‐Michel Rueff Pierre Rabu Carlo Massobrio Mauro Boero Alain Pautrat Paul‐Alain Jaffrès Guido Ori Guillaume Rogez 《Advanced functional materials》2017,27(41)
Copper‐ and cobalt‐based layered simple hydroxides (LSH) are successfully functionalized by a series of fluorene mono‐ and diphosphonic acids, using anionic exchange reactions and a preintercalation strategy. The lateral functionalization of the fluorene moieties has only little impact on the overall structure of the obtained layered hybrid materials but it influences the organization of the molecules within the interlamellar spacing. For bulky fluorene (9,9‐dioctyl derivative), luminescence is preserved when inserted into copper and cobalt hydroxydes, whereas it is completely quenched for the other fluorenes. Detailed characterization of the internal structure and chemical bonding properties for copper‐ and cobalt‐based hybrids is performed via ancillary experimental techniques. For the copper‐based LSH class, for which more elusive findings are found, first‐principles molecular dynamics simulations unravel the fundamental stabilizing role of the H‐bonding network promoted within the local environments of the fluorene mono‐ and diphosphonic acids. The cobalt series of compounds constitute a new class of hybrid magnets, with ordering temperatures ranging from 11.8 to 17.8 K and show a clear magnetoelectric effect. This effect appears above a threshold magnetic field, which is null below the magnetic ordering temperature, and it persists in the paramagnetic regime till about 110 K. 相似文献
998.
Gagey N Emond M Neveu P Benbrahim C Goetz B Aujard I Baudin JB Jullien L 《Organic letters》2008,10(12):2341-2344
This paper evaluates a series of photolabile protecting groups with built-in fluorescence reporting. They rely on readily available o-acetoxyphenyl methyloxazolones as activated precursors. Alcohol substrates are easily caged. The resulting photoactivable esters exhibit large one- and two-photon uncaging cross sections. The alcohol substrates are quantitatively released in a 1:1 molar ratio with a strongly fluorescent coumarin coproduct that serves as a reporter to quantify substrate delivery. 相似文献
999.
von Holst C Baeten V Boix A Slowikowski B Fernández Pierna JA Tirendi S Dardenne P 《Analytical and bioanalytical chemistry》2008,392(1-2):313-317
Near-infrared microscopy (NIRM) has been proved to be a powerful tool for the detection of banned meat and bone meal (MBM) in feed. The identification of MBM traces and its ability to differentiate animal from vegetable feed ingredients is based on the evaluation of near-infrared spectra obtained from individual particles present in the sample. This evaluation is supported by appropriate decision rules for the absorbances at specific wavelengths. Here we show that the method and the corresponding decision rules can be successfully transferred from the laboratory which constructed the decision rules to two independent laboratories that were not involved in the calibration process of the method. The analytical results from blind feed samples containing MBM (positive samples) and feed samples without MBM (negative samples) revealed a very good agreement between the three laboratories, thus demonstrating the transferability of the method. 相似文献
1000.
Following the isolation from marine sponges, in 1993, of a family of related highly oxygenated macrolactones named spongistatins, altohyrtins and cinachyrolides, impressive synthetic efforts have been devoted to the synthesis of these macrolides. Their highly potent activity as cancer cells growth inhibitors combined with a fascinating and complex architecture has prompted synthetic organic chemists to develop efficient routes to these molecules. From the first total syntheses by the groups of Evans and Kishi in 1997 and 1998 which delivered milligram quantities of spongistatins/altohyrtins, further intensive studies have led to new pathways with practical solution to provide gram scale amounts of key intermediates. The present review focuses on biological properties and synthetic issues related to these marine macrolides. 相似文献