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31.
32.
Coverage‐ and Temperature‐Dependent Metalation and Dehydrogenation of Tetraphenylporphyrin on Cu(111)
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Michael Röckert Matthias Franke Quratulain Tariq Stefanie Ditze Michael Stark Patrick Uffinger Daniel Wechsler Upendra Singh Dr. Jie Xiao Dr. Hubertus Marbach Prof. Dr. Hans‐Peter Steinrück Dr. Ole Lytken 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(29):8948-8953
Using temperature‐programmed desorption, supported by X‐ray photoelectron spectroscopy and scanning tunneling microscopy, a comprehensive overview of the main reactions of 5,10,15,20‐tetraphenyl‐21H,23H‐porphyrin (2HTPP) on Cu(111) as a function of coverage and temperature is obtained. Three reactions were identified: metalation with Cu substrate atoms, stepwise partial dehydrogenation, and finally complete dehydrogenation. At low coverage the reactions are independent of coverage, but at higher coverage metalation becomes faster and partial dehydrogenation slower. This behavior is explained by a weaker interaction between the iminic nitrogen atoms and the Cu(111) surface in the high‐coverage checkerboard structure, leading to faster metalation, and the stabilizing effect of T‐type interactions in the CuTPP islands formed at high coverage after metalation, leading to slower dehydrogenation. Based on the amount of hydrogen released and the appearance in STM, a structure of the partially dehydrogenated molecule is suggested. 相似文献
33.
Phosphine‐ and Hydrogen‐Free: Highly Regioselective Ruthenium‐Catalyzed Hydroaminomethylation of Olefins
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Dr. Samet Gülak Lipeng Wu Dr. Qiang Liu Prof. Dr. Robert Franke Dr. Ralf Jackstell Prof. Dr. Matthias Beller 《Angewandte Chemie (International ed. in English)》2014,53(28):7320-7323
A highly regioselective ruthenium‐catalyzed hydroaminomethylation of olefins is reported. Using easily available trirutheniumdodecacarbonyl an efficient sequence consisting of a water‐gas shift reaction, hydroformylation of olefins, with subsequent imine or enamine formation and final reduction is realized. This novel procedure is highly practical (ligand‐free, one pot) and economic (low catalyst loading and inexpensive metal). Bulk industrial as well as functionalized olefins react with various amines to give the corresponding tertiary amines generally in high yields (up to 92 %), excellent regioselectivities (n/iso>99:1), and full chemoselectivity in favor of terminal olefins. 相似文献
34.
Jiawang Liu Ji Yang Carolin Schneider Robert Franke Ralf Jackstell Matthias Beller 《Angewandte Chemie (International ed. in English)》2020,59(23):9032-9040
For the first time, the monoalkoxycarbonylation of easily available 1,3‐diynes to give synthetically useful conjugated enynes has been realized. Key to success was the design and utilization of the new ligand 2,2′‐bis(tert‐butyl(pyridin‐2‐yl)phosphanyl)‐1,1′‐binaphthalene (Neolephos), which permits the palladium‐catalyzed selective carbonylation under mild conditions, providing a general preparation of functionalized 1,3‐enynes in good‐to‐high yields with excellent chemoselectivities. Synthetic applications that showcase the possibilities of this novel methodology include an efficient one‐pot synthesis of 4‐aryl‐4H‐pyrans as well as the rapid construction of various heterocyclic, bicyclic, and polycyclic compounds. 相似文献
35.
Single element quasicrystalline monolayers were prepared by deposition of antimony and bismuth on the fivefold surface of icosahedral Al71.5Pd21Mn8.5 and the tenfold surface of decagonal Al71.8Ni14.8Co13.4. Elastic helium atom scattering and low energy electron diffraction of the monolayers show Bragg peaks at the bulk derived positions of the clean surfaces, revealing highly ordered quasicrystalline epitaxial films. Their adatom densities of (0.9+/-0.2)x10(15) cm(-2) and (0.8+/-0.2)x10(15) cm(-2) on Al-Pd-Mn and Al-Ni-Co, respectively, correspond to roughly one adatom per Al atom of the quasicrystalline substrate surfaces. 相似文献
36.
J. Rothe J. Pollmann R. Franke J. Hormes H. Bönnemann W. Brijoux K. Siepen J. Richter 《Fresenius' Journal of Analytical Chemistry》1996,355(3-4):372-374
Transition metal colloids are potential precursors of heterogeneous catalysts with application to selective chemical reactions. Sample preparation techniques are described. Experimental details are given of the characterization of these often air-sensitive particles by X-ray photoelectron and X-ray absorption spectroscopy. First results obtained with both techniques for a Rh-colloid show that the metal is mainly present in the zerovalent chemical state. But the spectra indicate further chemical states of Rh which can be assigned to the outermost metal atoms of the colloid interacting with organic ligands or to the educt Rh-halides. 相似文献
37.
38.
The preparation, properties and spectroscopic investigation (IR, 1H NMR, 31P NMR, MS) of η3-allyl[1,2-bis(diphenylphosphino)ethan]tricarbonylvanadium(0) compounds are reported. 相似文献
39.
The reaction of NaAsHR with ClCH2CH2CH2NH2 yields the corresponding secondary 3-aminopropylarsines, RAs(H)CH2CH2CH2NH2, which with aldehydes and ketones form the perhydro-1,3-azarsenines. The properties and reactivity of these heterocyclic compounds are described. 相似文献
40.
V.A. Franke 《Reports on Mathematical Physics》1980,18(3):411-431
An axiomatic scheme generalizing the operational approach to quantum theory is described. Only quite general axioms ensuring the existence of well-behaved probabilities are postulated. The space-time location of macroscopic apparatus interacting with the object is explicitly taken into consideration. The states and observables are defined and their time development is considered. The classification of physical processes with respect to their reversibility or irreversibility in time is given. The conditions of Lorentz and translational invariance are formulated. Linear transformations corresponding to operations on the object are introduced. In the case of reversible processes these transformations form an algebra and linear representations of the Poincaré group arise naturally. These results are, in general, invalid for irreversible processes. The position of quantum theory in the scheme described is clarified. 相似文献