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561.
Kai-Oliver Brenske Dr. Meike Emondts Sven T. Hörnig Sinan Panitz Maria I. Pieper Aron Ligori Alexander Schacht Johanna Henkel Prof. Dr. Jürgen Klankermayer Prof. Dr. Andreas Herrmann 《Angewandte Chemie (International ed. in English)》2023,62(22):e202300531
Enhancing NMR signals of biomacromolecules by hyperpolarization offers exciting opportunities for diagnostic applications. However, their hyperpolarization via parahydrogen remains challenging as specific catalytic interactions are required, which are difficult to tune due to the large size of the biomolecule and its insolubility in organic solvents. Herein, we show the unprecedented hyperpolarization of the cancer-targeting DNA aptamer AS1411. By screening different molecular motifs for an unsaturated label in nucleosides and in DNA oligomers, we were able to identify structural prerequisites for the hyperpolarization of AS1411. Finally, adjusting the polarity of AS1411 by complexing the DNA backbone with amino polyethylene glycol chains allowed the hydrogenation of the label with parahydrogen while the DNA structure remains stable to maintain its biological function. Our results are expected to advance hyperpolarized molecular imaging technology for disease detection in the future. 相似文献
562.
Ground rubber powder (GRP) with three different sizes was incorporated into nature rubber matrix with different loading. Cure characteristics, swelling behaviour, crosslink density, tensile fractured surface, and mechanical properties have been studied. Based on the cure characteristics, it is evident that the processability of the rubber compounds has not changed obviously with the different GRP loading. The introduction of GRP in virgin rubber leads to the increase in swelling degree and the decrease in crosslink density. Tensile strength, hardness and abrasion resistant deteriorate with the increase of GRP loading, but the tear resistance gets better. If the ground rubber particles are smaller, the properties are more similar to the virgin rubber. Because of the phase separation of the GRP and matrix, the properties get worse with the bigger ground rubber powder. 相似文献
563.
Ruxia Fan Dr. Johanna Hakanpää Karoliina Elfving Dr. Helena Taberman Prof. Markus B. Linder Dr. A. Sesilja Aranko 《Angewandte Chemie (International ed. in English)》2023,62(11):e202216371
A type of protein/peptide pair known as Catcher/Tag pair spontaneously forms an intermolecular isopeptide bond which can be applied for biomolecular click reactions. Covalent protein conjugation using Catcher/Tag pairs has turned out to be a valuable tool in biotechnology and biomedicines, but it is essential to increase the current toolbox of orthogonal Catcher/Tag pairs to expand the range of applications further, for example, for controlled multiple-fragment ligation. We report here the engineering of novel Catcher/Tag pairs for protein ligation, aided by a crystal structure of a minimal CnaB domain from Lactobacillus plantarum. We show that a newly engineered pair, called SilkCatcher/Tag enables efficient pH-inducible protein ligation in addition to being compatible with the widely used SpyCatcher/Tag pair. Finally, we demonstrate the use of the SilkCatcher/Tag pair in the production of native-sized highly repetitive spider-silk-like proteins with >90 % purity, which is not possible by traditional recombinant production methods. 相似文献
564.
Johanna Busch Thomas Niemann Jan Neumann Peter Stange Sabrina Gärtner Tristan Youngs Sarah Youngs Dr. Dietmar Paschek Dr. Ralf Ludwig 《Chemphyschem》2023,24(12):e202300031
Defects fundamentally govern the properties of all real materials. Correlating molecular defects to macroscopic quantities remains a challenge, particularly in the liquid phase. Herein, we report the influence of hydrogen bonds (HB) acting as defects in mixtures of non-hydroxyl-functionalized ionic liquids (ILs) with an increasing concentration of hydroxyl-functionalized ILs. We observed two types of HB defects: The conventional HBs between cation and anion (c–a), and the elusive HBs between cations (c–c) despite the repulsive Coulomb forces. We use neutron diffraction with isotopic substitution in combination with molecular dynamics simulations for measuring the geometry, strength, and distribution of mobile OH defects in the IL mixtures. In principle, this procedure allows relating the number and stability of defects to macroscopic properties such as diffusion, viscosity, and conductivity, which are of utmost importance for the performance of electrolytes in batteries and other electrical devices. 相似文献
565.
Jonas F. Goebel Johanna Stemmer Florian Belitz Lukas J. Gooßen 《Angewandte Chemie (International ed. in English)》2023,62(24):e202301839
The 3d-metal catalyst Mn(CO)5Br was found to efficiently promote ortho C−H allylations of arenecarboxylates in the presence of neocuproine as the ligand. Despite the simplicity of directing group and catalyst system, the selectivity goes well beyond the state-of-the-art in that mono-allylated products are obtained exclusively with high selectivities for the least hindered ortho-position. The directing group can optionally be removed by in situ decarboxylation, opening up a regioselective entry to allyl arenes. The preparative utility of the process and its othogonality to other approaches was demonstrated by 44 products with otherwise hard-to-access substitution patterns, including 3-bromo-allylbenzene, 3-allylbenzofuran, or 5-allyl-2-methylnitrobenzene. 相似文献
566.
Chenglong Luan Johanna Angona Arjun Bala Krishnan Manuel Corva Pouya Hosseini Markus Heidelmann Ulrich Hagemann Emmanuel Batsa Tetteh Wolfgang Schuhmann Kristina Tschulik Tong Li 《Angewandte Chemie (International ed. in English)》2023,62(28):e202305982
The role of β-CoOOH crystallographic orientations in catalytic activity for the oxygen evolution reaction (OER) remains elusive. We combine correlative electron backscatter diffraction/scanning electrochemical cell microscopy with X-ray photoelectron spectroscopy, transmission electron microscopy, and atom probe tomography to establish the structure–activity relationships of various faceted β-CoOOH formed on a Co microelectrode under OER conditions. We reveal that ≈6 nm β-CoOOH(01 0), grown on [ 0]-oriented Co, exhibits higher OER activity than ≈3 nm β-CoOOH(10 3) or ≈6 nm β-CoOOH(0006) formed on [02 - and [0001]-oriented Co, respectively. This arises from higher amounts of incorporated hydroxyl ions and more easily reducible CoIII−O sites present in β-CoOOH(01 0) than those in the latter two oxyhydroxide facets. Our correlative multimodal approach shows great promise in linking local activity with atomic-scale details of structure, thickness and composition of active species, which opens opportunities to design pre-catalysts with preferred defects that promote the formation of the most active OER species. 相似文献