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111.
Control of the Electronic Ground State on an Electron‐Transfer Copper Site by Second‐Sphere Perturbations 下载免费PDF全文
Marcos N. Morgada Dr. Luciano A. Abriata Ulises Zitare Dr. Damian Alvarez‐Paggi Prof. Daniel H. Murgida Prof. Alejandro J. Vila 《Angewandte Chemie (International ed. in English)》2014,53(24):6188-6192
The CuA center is a dinuclear copper site that serves as an optimized hub for long‐range electron transfer in heme–copper terminal oxidases. Its electronic structure can be described in terms of a σu* ground‐state wavefunction with an alternative, less populated ground state of πu symmetry, which is thermally accessible. It is now shown that second‐sphere mutations in the CuA containing subunit of Thermus thermophilus ba3 oxidase perturb the electronic structure, which leads to a substantial increase in the population of the πu state, as shown by different spectroscopic methods. This perturbation does not affect the redox potential of the metal site, and despite an increase in the reorganization energy, it is not detrimental to the electron‐transfer kinetics. The mutations were achieved by replacing the loops that are involved in protein–protein interactions with cytochrome c, suggesting that transient protein binding could also elicit ground‐state switching in the oxidase, which enables alternative electron‐transfer pathways. 相似文献
112.
Pastor E Matveeva E Valle-Gallego A Goycoolea FM Garcia-Fuentes M 《Colloids and surfaces. B, Biointerfaces》2011,88(2):601-609
Mesoporous silicon is a biocompatible, biodegradable material that is receiving increased attention for pharmaceutical applications due to its extensive specific surface. This feature enables to load a variety of drugs in mesoporous silicon devices by simple adsorption-based procedures. In this work, we have addressed the fabrication and characterization of two new mesoporous silicon devices prepared by electrochemistry and intended for protein delivery, namely: (i) mesoporous silicon microparticles and (ii) chitosan-coated mesoporous silicon microparticles. Both carriers were investigated for their capacity to load a therapeutic protein (insulin) and a model antigen (bovine serum albumin) by adsorption. Our results show that mesoporous silicon microparticles prepared by electrochemical methods present moderate affinity for insulin and high affinity for albumin. However, mesoporous silicon presents an extensive capacity to load both proteins, leading to systems were protein could represent the major mass fraction of the formulation. The possibility to form a chitosan coating on the microparticles surface was confirmed both qualitatively by atomic force microscopy and quantitatively by a colorimetric method. Mesoporous silicon microparticles with mean pore size of 35 nm released the loaded insulin quickly, but not instantaneously. This profile could be slowed to a certain extent by the chitosan coating modification. With their high protein loading, their capacity to provide a controlled release of insulin over a period of 60-90 min, and the potential mucoadhesive effect of the chitosan coating, these composite devices comprise several features that render them interesting candidates as transmucosal protein delivery systems. 相似文献
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Marcos Rosenbaum 《International Journal of Theoretical Physics》2001,40(1):139-163
Connes' noncommutative geometry is presented and the relevance of the Dirac operator in the elucidation of the structure of space-time at the Planck length is discussed. 相似文献
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Richard P. Brinn Jaydione Marcon Marcos Tavares-Dias Ira M. Brinn 《Photochemistry and photobiology》2009,85(1):358-364
The fluorescence spectra of the tropical fish, Cardinal Tetra ( Paracheirodon axelrodi ), originating in the Amazon region of Brazil, were determined. These spectra were then treated using factor analysis, generating two contributing spectra and separating out the noise. Time-resolved fluorescence results indicated that the fluorescent system in the epidermis undergoes excited state reaction. Excited state proton transfer is suggested as being present. Both intentionally stressed and nonstressed individuals were used and some small differences were noted in the contributions of the two calculated contributing spectra to the experimental spectra, presumably as a function of stress. The results are compared with those obtained by the standard determination of cortisol level using the whole body extraction method and it is suggested that the method could be tested as an improved, nondestructive way to determine stress in this species, which is a necessary step in the development of "best management practices" of methods for storage and transport of the fish. 相似文献
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Sônia Cristina Poltroniere Kelly Cristina Poldi Franklina Maria Bragion Toledo Marcos Nereu Arenales 《Annals of Operations Research》2008,157(1):91-104
An important production programming problem arises in paper industries coupling multiple machine scheduling with cutting stocks.
Concerning machine scheduling: how can the production of the quantity of large rolls of paper of different types be determined.
These rolls are cut to meet demand of items. Scheduling that minimizes setups and production costs may produce rolls which
may increase waste in the cutting process. On the other hand, the best number of rolls in the point of view of minimizing
waste may lead to high setup costs. In this paper, coupled modeling and heuristic methods are proposed. Computational experiments
are presented. 相似文献