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141.
Alois Pfenniger Andreas Stahel Volker M. Koch Dominik Obrist Rolf Vogel 《Applied Mathematical Modelling》2014
Engineers are confronted with the energy demand of active medical implants in patients with increasing life expectancy. Scavenging energy from the patient’s body is envisioned as an alternative to conventional power sources. Joining in this effort towards human-powered implants, we propose an innovative concept that combines the deformation of an artery resulting from the arterial pressure pulse with a transduction mechanism based on magneto-hydrodynamics. To overcome certain limitations of a preliminary analytical study on this topic, we demonstrate here a more accurate model of our generator by implementing a three-dimensional multiphysics finite element method (FEM) simulation combining solid mechanics, fluid mechanics, electric and magnetic fields as well as the corresponding couplings. This simulation is used to optimize the generator with respect to several design parameters. A first validation is obtained by comparing the results of the FEM simulation with those of the analytical approach adopted in our previous study. With an expected overall conversion efficiency of 20% and an average output power of 30 μW, our generator outperforms previous devices based on arterial wall deformation by more than two orders of magnitude. Most importantly, our generator provides sufficient power to supply a cardiac pacemaker. 相似文献
142.
Dr. Dominique T. Thielemann Anna T. Wagner Dr. Yanhua Lan Dr. Pascual Oña‐Burgos Prof. Dr. Ignacio Fernández Prof. Dr. Esther S. Rösch Dr. Dominik K. Kölmel Prof. Dr. Annie K. Powell Prof. Dr. Stefan Bräse Prof. Dr. Peter W. Roesky 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(7):2813-2820
A new family of pentadecanuclear coordination cluster compounds (from now on simply referred to as clusters) [{Ln15(OH)20(PepCO2)10(DBM)10Cl}Cl4] (PepCO2=2‐[{3‐(((tert‐butoxycarbonyl)amino)methyl)benzyl}amino]acetate, DBM=dibenzoylmethanide) with Ln=Y and Dy was obtained by using the cell‐penetrating peptoid (CPPo) monomer PepCO2H and dibenzoylmethane (DBMH) as supporting ligands. The combination of an inorganic cluster core with an organic cell‐penetrating peptoid in the coordination sphere resulted in a core component {Ln15(μ3‐OH)20Cl}24+ (Ln=Y, Dy), which consists of five vertex‐sharing heterocubane {Ln4(μ3‐OH)4}8+ units that assemble to give a pentagonal cyclic structure with one Cl atom located in the middle of the pentagon. The solid‐state structures of both clusters were established by single‐crystal X‐ray crystallography. MS (ESI) experiments suggest that the cluster core is robust and maintained in solution. Pulsed gradient spin echo (PGSE) NMR diffusion measurements were carried out on the diamagnetic yttrium compound and confirmed the stability of the cluster in its dicationic form [{Y15(μ3‐OH)20(PepCO2)10(DBM)10Cl}Cl2]2+. The investigation of both static (dc) and dynamic (ac) magnetic properties in the dysprosium cluster revealed a slow relaxation of magnetization, indicative of single‐molecule magnet (SMM) behavior below 8 K. Furthermore, the χT product as a function of temperature for the dysprosium cluster gave evidence that this is a ferromagnetically coupled compound below 11 K. 相似文献
143.
Saeed Amirjalayer Harald Fuchs Dominik Marx 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(16):5286-5289
On the way to establishing biomass as a renewable and environmentally friendly source to cover the ever‐increasing global demand on energy and chemicals, one great challenge is the efficient depolymerization of cellulose. Enhanced conversion rates have been discovered in ball‐milling experiments, thus opening a mechanocatalytic approach. However, an understanding of the impact of mechanical forces on the acid‐catalyzed cleavage of glycosidic bonds at the molecular level is still missing. Herein, we contribute such fundamental insight based on atomistic modeling. Mechanically stressing the macromolecular backbone radically changes the depolymerization pathway from a complex high‐barrier reaction upon thermal activation to a low‐energy single‐step mechanocatalytic process. In addition to revealing a regioselective increase in basicity under a mechanical force, our results provide molecular‐level explanations of the experimental findings and might therefore guide rational ways to improve such mechanocatalytic processes. 相似文献
144.
Tobias Ullrich Piermaria Pinter Julian Messelberger Philipp Haines Ramandeep Kaur Jun.-Prof. Dr. Max M. Hansmann Dr. Dominik Munz Prof. Dr. Dirk M. Guldi 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(20):7980-7988
Herein, we present a new class of singlet fission (SF) materials based on diradicaloids of carbene scaffolds, namely cyclic (alkyl)(amino)carbenes (CAACs). Our modular approach allows the tuning of two key SF criteria: the steric factor and the diradical character. In turn, we modified the energy landscapes of excited states in a systematic manner to accommodate the needs for SF. We report the first example of intermolecular SF in solution by dimer self-assembly at cryogenic temperatures. 相似文献
145.
Dominik Schauenburg Dr. Mohammad Divandari Dr. Kevin Neumann Christoph A. Spiegel Thomas Hackett Yi-Chung Dzeng Prof. Dr. Nicholas D. Spencer Prof. Dr. Jeffrey W. Bode 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(34):14764-14771
We report the synthesis of monomers for atom-transfer radical polymerization (ATRP) and a reversible addition-fragmentation chain transfer (RAFT) agent bearing trifluoroborate iminiums (TIMs), which are quantitatively converted into potassium acyltrifluoroborates (KATs) after polymerization. The resulting KAT-containing polymers are suitable for rapid amide-forming ligations for both post-polymerization modification and polymer conjugation. The polymer conjugation occurs rapidly, even under dilute (micromolar) aqueous conditions at ambient temperatures, thereby enabling the synthesis of a variety of linear and star-shaped block copolymers. In addition, we applied post-polymerization modification to the covalent linking of a photocaged cyclic antibiotic (gramicidin S) to the side chains of the KAT-containing copolymer. Cellular assays revealed that the polymer–antibiotic conjugate is biocompatible and provides efficient light-controlled release of the antibiotic on demand. 相似文献
146.
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148.
This paper presents a framework for incorporating arbitrary implicit multistep schemes into the lattice Boltzmann method. While the temporal discretization of the lattice Boltzmann equation is usually derived using a second-order trapezoidal rule, it appears natural to augment the time discretization by using multistep methods. The effect of incorporating multistep methods into the lattice Boltzmann method is studied in terms of accuracy and stability. Numerical tests for the third-order accurate Adams-Moulton method and the second-order backward differentiation formula show that the temporal order of the method can be increased when the stability properties of multistep methods are considered in accordance with the second Dahlquist barrier. 相似文献
149.
Combination of molecular dynamics simulations and miscibility calculations was used to investigate erlotinib drug delivery systems based on poly-ε-caprolactone–polyethylene glycol–poly-ε-caprolactone (PCL–PEG–PCL) and poly-ε-caprolactone–polyglycolic acid–poly-ε-caprolactone (PCL–PGA–PCL) biodegradable copolymers. The molecular modeling strategy involving visual observation of models, concentration profile analysis, Flory–Huggins χ parameter, cohesive energy density, and mean square displacement calculations reproduced experimental evidence of erlotinib release from PCL–PEG–PCL matrix successfully. Increasing portion of PCL in PCL–PEG–PCL copolymer led to dissolution of erlotinib aggregates recorded in visual and concentration profile analyses. Higher portion of PCL led to higher cohesive energy density and lower mean square displacement values. Success of this strategy in reproduction of experimental data made an opportunity to utilize the same modeling design in prediction of erlotinib release from similar but not yet experimentally tested PCL–PGA–PCL matrix. In this case, agglomeration of erlotinib molecules and stronger cohesive energy density values were observed. 相似文献
150.
Access to the Bis‐benzene Cobalt(I) Sandwich Cation and its Derivatives: Synthons for a “Naked” Cobalt(I) Source?
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Stefan C. Meier Albina Holz Jan Kulenkampff Alexei Schmidt Dr. Daniel Kratzert Dr. Daniel Himmel Dominik Schmitz Dr. Ernst‐Wilhelm Scheidt Prof. Dr. Wolfgang Scherer Dr. Christine Bülow Martin Timm Dr. Rebecka Lindblad Dr. Scott T. Akin Dr. Vicente Zamudio‐Bayer Prof. Dr. Bernd von Issendorff Prof. Dr. Michael A. Duncan Prof. Dr. J. Tobias Lau Prof. Dr. Ingo Krossing 《Angewandte Chemie (International ed. in English)》2018,57(30):9310-9314
The synthesis and structural characterization of the hitherto unknown parent Co(bz)2+ (bz=benzene) complex and several of its derivatives are described. Their synthesis starts either from a CoCO5+ salt, or directly from Co2(CO)8 and a Ag+ salt. Stability and solubility of these complexes was achieved by using the weakly coordinating anions (WCAs) [Al(ORF)4]? and [F{Al(ORF)3}2]? {RF=C(CF3)3} and the solvent ortho‐difluorobenzene (o‐DFB). The magnetic properties of Co(bz)2+ were measured and compared in the condensed and gas phases. The weakly bound Co(o‐dfb)2+ salts are of particular interest for the preparation of further CoI salts, for example, the structurally characterized low‐coordinate 12 valence electron Co(PtBu3)2+ and Co(NHC)2+ salts. 相似文献