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31.
The influence of thermal fluctuations on the dynamics of interfacial electron transfer in sensitized TiO2-anatase semiconductors is investigated by combining ab initio DFT molecular dynamics simulations and quantum dynamics propagation of transient electronic excitations. It is shown that thermal nuclear fluctuations speed up the underlying interfacial electron transfer dynamics by introducing nonadiabatic transitions between electron acceptor states, localized in the vicinity of the photoexcited adsorbate, and delocalized states extended throughout the semiconductor material, creating additional relaxation pathways for carrier diffusion. Furthermore, it is shown that room-temperature thermal fluctuations reduce the anisotropic character of charge diffusion along different directions in the anatase crystal and make similar the rates for electron injection from adsorbate states of different character. The reported results are particularly relevant to the understanding of temperature effects on surface charge separation mechanisms in molecular-based photo-optic devices. 相似文献
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Luiz Carlos Domingos Batista Thiago Izidoro Silva Santos José E. Lima Santos Djalma Ribeiro da Silva Carlos A. Martínez-Huitle 《Electroanalysis》2021,33(1):57-65
MOF-235 is presented as an orange powder, with crystals of the octahedral formation. It was already used as adsorbent to remove different compounds from water; however, no attempts have been published about the exploration of the MOF-235 application as electrochemical sensor for organic compounds yet. MOF-235 was synthetized and after that, it was characterized by SEM, XRD and FTIR. Graphite electrodes (GEs) were modified with different MOF-235 ratio (5 %, 7 %, 10 %, 12 % and 14 %) and these modified GEs were characterized by cyclic voltammetry (CV) measurements in order to determine the effect of MOF-235 concentration on the current response. Results indicated that, a significant improvement on the current response was attained at MOF-235(10 %)/GE respect to unmodified GE. This behavior is related to the pore structure and multiple active sites on the MOF surface. The performance of the MOF-235(10 %)/GE as electrochemical sensor for detecting catechol was assessed by differential pulse voltammetry (DPV). Catechol detection response of MOF-based sensor provided a detection limit of about 12.79 μmol L−1 with a correlation coefficient (R2) of about 0.9928 ranging from 12 to 514 μmol L−1. Finally, MOF-235(10 %)/GE was used to determine catechol in real water matrixes. 相似文献
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Trifluoroacetamide is easily monoalkylated in a K2 CO3-organic solvent solid-liquid two-phase system affording in good to excellent yields N-alkyltrifluoroacetamides. Under the same conditions, the latter, in turn, react with alkylating agents giving N, N-dialkyltrifluoroacetamides in high yields. 相似文献
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Vito Dario Camiola Giovanni Mascali Vittorio Romano 《Continuum Mechanics and Thermodynamics》2012,24(4-6):417-436
A nanoscale double-gate MOSFET is simulated with an energy-transport subband model for semiconductors formulated starting from the moment system derived from the Schr?dinger–Poisson–Boltzmann equations. The system is closed on the basis of the maximum entropy principle and includes scattering of electrons with acoustic and non-polar optical phonons. The proposed expression of the entropy combines quantum effects and semiclassical transport by weighting the contribution of each subband with the square modulus of the envelope functions arising from the Schr?dinger–Poisson subsystem. The simulations show that the model is able to capture the relevant confining and transport features and assess the robustness of the numerical scheme. 相似文献
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Hydroxyl Radical Generation and DNA Nuclease Activity: A Mechanistic Study Based on a Surface‐Immobilized Copper Thioether Clip‐Phen Derivative
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Adolfo I. B. Romo Dieric S. Abreu Dr. Tércio de F. Paulo Dr. Marta S. P. Carepo Prof. Eduardo H. S. Sousa Prof. Luis Lemus Prof. Carolina Aliaga Prof. Alzir A. Batista Prof. Otaciro R. Nascimento Prof. Héctor D. Abruña Prof. Izaura C. N. Diógenes 《Chemistry (Weinheim an der Bergstrasse, Germany)》2016,22(29):10081-10089
Coordination compounds of copper have been invoked as major actors in processes involving the reduction of molecular oxygen, mostly with the generation of radical species the assignment for which has, so far, not been fully addressed. In the present work, we have carried out studies in solution and on surfaces to gain insights into the nature of the radical oxygen species (ROS) generated by a copper(II) coordination compound containing a thioether clip‐phen derivative, 1,3‐bis(1,10‐phenanthrolin‐2‐yloxy)‐N‐(4‐(methylthio)benzylidene)propan‐2‐amine (2CP‐Bz‐SMe), enabling its adsorption/immobilization to gold surfaces. Whereas surface plasmon resonance (SPR) and electrochemistry of the adsorbed complex indicated the formation of a dimeric CuI intermediate containing molecular oxygen as a bridging ligand, scanning electrochemical microscopy (SECM) and nuclease assays pointed to the generation of a ROS species. Electron paramagnetic resonance (EPR) data reinforced such conclusions, indicating that radical production was dependent on the amount of oxygen and H2O2, thus pointing to a mechanism involving a Fenton‐like reaction that results in the production of OH.. 相似文献
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Ricerche di Matematica - This paper provides an account of results and methods from the theory of infinite groups admitting only finitely many normalizers of subgroups with a given property. Some... 相似文献