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311.
This paper generalizes Shelah’s generic pair conjecture (now theorem) for the measurable cardinal case from first order theories to finite diagrams. We use homogeneous models in the place of saturated models. 相似文献
312.
Verena I. Böhmer Prof. Wiktor Szymanski Keimpe-Oeds van den Berg Chantal Mulder Piermichele Kobauri Hugo Helbert Dr. Dion van der Born Friederike Reeβing Anja Huizing Dr. Marten Klopstra Douwe F. Samplonius Dr. Ines F. Antunes Jürgen W. A. Sijbesma Dr. Gert Luurtsema Prof. Wijnand Helfrich Dr. Ton J. Visser Prof. Ben L. Feringa Prof. Philip H. Elsinga 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(47):10871-10881
Since the seminal contribution of Rolf Huisgen to develop the [3+2] cycloaddition of 1,3-dipolar compounds, its azide–alkyne variant has established itself as the key step in numerous organic syntheses and bioorthogonal processes in materials science and chemical biology. In the present study, the copper(I)-catalyzed azide–alkyne cycloaddition was applied for the development of a modular molecular platform for medical imaging of the prostate-specific membrane antigen (PSMA), using positron emission tomography. This process is shown from molecular design, through synthesis automation and in vitro studies, all the way to pre-clinical in vivo evaluation of fluorine-18- labeled PSMA-targeting ‘F-PSMA-MIC’ radiotracers (t1/2=109.7 min). Pre-clinical data indicate that the modular PSMA-scaffold has similar binding affinity and imaging properties to the clinically used [68Ga]PSMA-11. Furthermore, we demonstrated that targeting the arene-binding in PSMA, facilitated through the [3+2]cycloaddition, can improve binding affinity, which was rationalized by molecular modeling. The here presented PSMA-binding scaffold potentially facilitates easy coupling to other medical imaging moieties, enabling future developments of new modular imaging agents. 相似文献
313.
Lucas Wäschenbach Christoph G. W. Gertzen Verena Keitel Holger Gohlke 《Journal of computational chemistry》2020,41(9):874-884
We describe the first extensive energetic evaluation of GPCR dimerization on the atomistic level by means of potential of mean force (PMF) computations and implicit solvent/implicit membrane end-point free energy calculations (MM-PBSA approach). Free energies of association computed from the PMFs show that the formation of both the 1/8 and 4/5 interface is energetically favorable for TGR5, the first GPCR known to be activated by hydrophobic bile acids and neurosteroids. Furthermore, formation of the 1/8 interface is favored over that of the 4/5 interface. Both results are in line with our previous FRET experiments in live cells. Differences in lipid-protein interactions are identified to contribute to the observed differences in free energies of association. A per-residue decomposition of the MM-PBSA effective binding energy reveals hot spot residues specific for both interfaces that form clusters. This knowledge may be used to guide the design of dimerization inhibitors or perform mutational studies to explore physiological consequences of distorted TGR5 association. Finally, we characterized the role of Y111, located in the conserved (D/E)RY motif, as a facilitator of TGR5 interactions. The types of computations performed here should be transferable to other transmembrane proteins that form dimers or higher oligomers as long as good structural models of the dimeric or oligomeric states are available. Such computations may help to overcome current restrictions due to an imperfect energetic representation of protein association at the coarse-grained level. © 2019 The Authors. Journal of Computational Chemistry published by Wiley Periodicals LLC. 相似文献
314.
315.
Norihiro Tokitoh Verena Stresing Yasusuke Matsuhashi Renji Okazaki 《Heteroatom Chemistry》1995,6(2):155-160
Reactions of a sterically crowded 1,3,2-dithiastannetane derivative bearing 2,4,6-tris[bis(trimethylsilyl)methyl]phenyl (=Tbt) and 2,4,6-triisopropylphenyl (=Tip) groups on the tin atom are described. Both thermolysis and photolysis of the 1,3,2-dithiastannetane [Tbt(Tip)SnS2CPh2] resulted in the formation of products derived from the corresponding stannanethione [Tbt(Tip)Sn=S], while the oxidation reaction by m -chloroperbenzoic acid gave a novel tincontaining heterocyclic system, an 1,2,4,5-oxadithiastannolane derivative. 相似文献