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排序方式: 共有240条查询结果,搜索用时 31 毫秒
1.
Giuseppe Spedalotto Dr. Robert Gericke Marta Lovisari Dr. Erik R. Farquhar Dr. Brendan Twamley Dr. Aidan R. McDonald 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(51):11983-11990
Hydroxide-bridged high-valent oxidants have been implicated as the active oxidants in methane monooxygenases and other oxidases that employ bimetallic clusters in their active site. To understand the properties of such species, bis-μ-hydroxo-NiII2 complex ( 1 ) supported by a new dicarboxamidate ligand (N,N′-bis(2,6-dimethyl-phenyl)-2,2-dimethylmalonamide) was prepared. Complex 1 contained a diamond core made up of two NiII ions and two bridging hydroxide ligands. Titration of the 1 e− oxidant (NH4)2[CeIV(NO3)6] with 1 at −45 °C showed the formation of the high-valent species 2 and 3 , containing NiIINiIII and NiIII2 diamond cores, respectively, maintaining the bis-μ-hydroxide core. Both complexes were characterised using electron paramagnetic resonance, X-ray absorption, and electronic absorption spectroscopies. Density functional theory computations supported the spectroscopic assignments. Oxidation reactivity studies showed that bis-μ-hydroxide-NiIII2 3 was capable of oxidizing substrates at −45 °C at rates greater than that of the most reactive bis-μ-oxo-NiIII complexes reported to date. 相似文献
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A. Brandl M. Pfitzner J. D. Mooney B. Durst W. Kern 《Flow, Turbulence and Combustion》2005,75(1-4):335-350
In order to simulate the turbulent combustion process occurring in spark-ignition (IC) engines, it is necessary to provide
suitable and numerically economical models, the latter being particularly important in the application to industrial problems.
Moreover, these models must deliver sufficiently accurate results for the unsteady operation of spark combustion engines,
concerning variable geometries, temperatures, pressures and charge development in different configurations. In this work different
turbulent combustion models for premixed hydrocarbon combustion are compared with respect to their ability to accurately predict
the propagation of turbulent perfectly premixed flames.
As a first configuration a cylinder of constant volume was studied. Transient calculations were used to simulate the propagation
of the turbulent flame and to evaluate the resulting turbulent burning velocity. These calculations were performed for a perfect
mixture of air and hydrocarbons at stoichiometric mixture and different initial conditions concerning pressure, temperature
and turbulence intensity. As a second configuration a stationary turbulent bunsen-type flame with methane fuel was used to
validate the turbulent combustion model of [Lindstedt and Vaos, Combust. Flame 116 (1999) 461] at different pressures. Calculated results were then compared to experimental data of [Kobayashi, Tamura,
Maruta and Niioka. In: Proceedings of the 26th Symposium on Combustion, 1996, p. 389] and show excellent agreement for the turbulent burning velocity at several pressure levels using only a single
set of model parameters. 相似文献
4.
Connor Mooney 《偏微分方程通讯》2019,44(8):681-690
5.
Xin Chen Aleksandra M. Krajewska Dr. Cormac McGuinness Amy Lynes David McAteer Nina Berner Prof. Georg Duesberg Prof. Jonathan N. Coleman Prof. Aidan R. McDonald 《Chemistry (Weinheim an der Bergstrasse, Germany)》2021,27(3):984-992
Covalently tethering photosensitizers to catalytically active 1T-MoS2 surfaces holds great promise for the solar-driven hydrogen evolution reaction (HER). Herein, we report the preparation of two new RuII-complex-functionalized MoS2 hybrids [RuII(bpy)2(phen)]-MoS2 and [RuII(bpy)2(py)Cl]-MoS2. The influence of covalent functionalization of chemically exfoliated 1T-MoS2 with coordinating ligands and RuII complexes on the HER activity and photo-electrochemical performance of this dye-sensitized system was studied systematically. We find that the photo-electrochemical performance of this RuII-complex-sensitized MoS2 system is highly dependent on the surface extent of photosensitizers and the catalytic activity of functionalized MoS2. The latter was strongly affected by the number and the kind of functional groups. Our results underline the tunability of the photovoltage generation in this dye-sensitized MoS2 system by manipulation of the surface functionalities, which provides a practical guidance for smart design of future dye-sensitized MoS2 hydrogen production devices towards improved the photofuel conversion efficiency. 相似文献
6.
Characterising the metric and topological evolution of OpenStreetMap network representations 总被引:3,自引:0,他引:3
OpenStreetMap (OSM) is a collaborative project to create a free editable map database of the world. This paper presents an analysis of the evolution of OSM street network representations. Three urban areas in Ireland were analysed where each evolves from containing little street network detail to a highly detailed street network. In order to characterise this evolution a number of metric and topological characteristics were computed. Some characteristics exhibited broadly similar behaviour in each region. This may be a attributed to similarities in the degree of contributor activity and intrinsic universal mapping procedures exhibited by contributors. 相似文献
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We prove that every Kirchberg algebra in the UCT class has nuclear dimension 1. We first show that Kirchberg 2-graph algebras with trivial K0 and finite K1 have nuclear dimension 1 by adapting a technique developed by Winter and Zacharias for Cuntz algebras. We then prove that every Kirchberg algebra in the UCT class is a direct limit of 2-graph algebras to obtain our main theorem. 相似文献
10.
The large intrinsic band gap of NiO has hindered severely its potential application under visible-light irradiation. In this Letter, we have performed first-principles calculations on the electronic properties of N- and C-doped NiO to ascertain if its band gap may be narrowed theoretically. It was found that impurity bands driven by N 2p or C 2p states appear in the band gap of NiO and that some of these locate at the conduction band minimum, which leads to a significant band gap narrowing. Our results show that N-doped NiO may serve as a potential photocatalyst relative to C-doped NiO, due to the presence of some recombination centres in C-doped NiO. 相似文献