全文获取类型
收费全文 | 328篇 |
免费 | 38篇 |
国内免费 | 1篇 |
专业分类
化学 | 331篇 |
晶体学 | 1篇 |
力学 | 4篇 |
数学 | 4篇 |
物理学 | 27篇 |
出版年
2023年 | 5篇 |
2022年 | 5篇 |
2021年 | 5篇 |
2020年 | 6篇 |
2019年 | 9篇 |
2018年 | 3篇 |
2017年 | 6篇 |
2016年 | 18篇 |
2015年 | 15篇 |
2014年 | 10篇 |
2013年 | 18篇 |
2012年 | 24篇 |
2011年 | 28篇 |
2010年 | 13篇 |
2009年 | 8篇 |
2008年 | 21篇 |
2007年 | 18篇 |
2006年 | 23篇 |
2005年 | 26篇 |
2004年 | 19篇 |
2003年 | 16篇 |
2002年 | 21篇 |
2001年 | 5篇 |
2000年 | 2篇 |
1999年 | 5篇 |
1998年 | 3篇 |
1997年 | 2篇 |
1996年 | 6篇 |
1995年 | 4篇 |
1994年 | 3篇 |
1993年 | 2篇 |
1992年 | 1篇 |
1991年 | 2篇 |
1990年 | 1篇 |
1987年 | 1篇 |
1985年 | 1篇 |
1984年 | 3篇 |
1983年 | 2篇 |
1982年 | 3篇 |
1980年 | 2篇 |
1977年 | 1篇 |
1975年 | 1篇 |
排序方式: 共有367条查询结果,搜索用时 31 毫秒
41.
Synergic Catalysis of PdCu Alloy Nanoparticles within a Macroreticular Basic Resin for Hydrogen Production from Formic Acid 下载免费PDF全文
Prof. Dr. Kohsuke Mori Dr. Hiromasa Tanaka Masahiro Dojo Prof. Dr. Kazunari Yoshizawa Prof. Dr. Hiromi Yamashita 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(34):12085-12092
Highly dispersed PdCu alloy nanoparticles have been successfully prepared within a macroreticular basic resin bearing ?N(CH3)2 functional groups. This previously unappreciated combination of alloy is first proven to be responsible for the efficient production of high‐purity H2 from formic acid (HCOOH) dehydrogenation for chemical hydrogen storage. By the addition of Cu, the electronically promoted Pd sites show significantly higher catalytic activity as well as a better tolerance towards CO poisoning as compared to their monometallic Pd counterparts. Experimental and DFT calculation studies revealed not only the synergic alloying effect but also cooperative action by the ?N(CH3)2 groups within the resin play crucial roles in achieving exceptional catalytic performances. In addition to the advantages such as, facile preparation method, free of additives, recyclable without leaching of active component, and suppression of unfavorable CO formation less than 3 ppm, the present catalytic system is cost‐effective because of the superior catalytic activity compared with that of well‐established precious PdAg or PdAu catalysts. The present catalytic system is particularly desirable for an ideal hydrogen vector in terms of potential industrial application for fuel cells. 相似文献
42.
43.
Taniguchi M Tsutsui M Mogi R Sugawara T Tsuji Y Yoshizawa K Kawai T 《Journal of the American Chemical Society》2011,133(30):11426-11429
The symmetry of a molecule junction has been shown to play a significant role in determining the conductance of the molecule, but the details of how conductance changes with symmetry have heretofore been unknown. Herein, we investigate a naphthalenedithiol single-molecule system in which sulfur atoms from the molecule are anchored to two facing gold electrodes. In the studied system, the highest single-molecule conductance, for a molecule junction of 1,4-symmetry, is 110 times larger than the lowest single-molecule conductance, for a molecule junction of 2,7-symmetry. We demonstrate clearly that the measured dependence of molecule junction symmetry for single-molecule junctions agrees with theoretical predictions. 相似文献
44.
We examined two-dimensional (2D) optical feedback control of phototaxis flagellate Euglena cells confined in closed-type microfluidic channels (microaquariums), and demonstrated that the 2D optical feedback enables the control of the density and position of Euglena cells in microaquariums externally, flexibly, and dynamically. Using three types of feedback algorithms, the density of Euglena cells in a specified area can be controlled arbitrarily and dynamically, and more than 70% of the cells can be concentrated into a specified area. Separation of photo-sensitive/insensitive Euglena cells was also demonstrated. Moreover, Euglena-based neuro-computing has been achieved, where 16 imaginary neurons were defined as Euglena-activity levels in 16 individual areas in microaquariums. The study proves that 2D optical feedback control of photoreactive flagellate microbes is promising for microbial biology studies as well as applications such as microbe-based particle transportation in microfluidic channels or separation of photo-sensitive/insensitive microbes. 相似文献
45.
46.
Yokoi T Sakuma J Maeda K Domen K Tatsumi T Kondo JN 《Physical chemistry chemical physics : PCCP》2011,13(7):2563-2570
The confined space synthesis method has been applied to the preparation of sodium tantalate (NaTaO(3)); hydrothermal reaction of NaOH and Ta(2)O(5) was carried out in the pores of a three-dimensional mesoporous carbon, which was replicated by the colloidal array of silica nanospheres (SNSs) 20 nm in size. This approach led to the formation of a colloidal array of NaTaO(3) nanoparticles 20 nm in size with a surface area of 34 m(2) g(-1). The photocatalytic performance of the colloidal array of NaTaO(3) nanoparticles for overall water splitting under UV irradiation (λ > 200 nm) was evaluated after loading a NiO cocatalyst onto NaTaO(3) samples. The NiO-loaded NaTaO(3) nanoparticles showed photocatalytic activity for overall water splitting more than three times as high as non-structured bulk NaTaO(3) particles. 相似文献
47.
The basic characteristics of vaporization and flowing behavior of n-pentane injected through a single nozzle into a column of hot water have been studied photographically. Subcools at the nozzle-outlet have a strong influence on the critical temperature driving forces at over which vaporization can be maintained. The length of a Rayleigh jet is remarkably shortened when vaporization occurs, whereas mean diameters of drops are little affected whether vaporization occurs or not. A specific condition that a bubble appears in each drop is satisfied not on a specific line but over a wide region on the ΔT∞ - UN plane. 相似文献
48.
Kazunari Ohgaki Susumu Nakai Satoshi Nitta Takashi Katayama 《Fluid Phase Equilibria》1982,8(2):113-122
isothermal vapor-liquid equilibria for the binary systems propylene-carbon dioxide, propylene-ethylene and propylene-ethane have been measured at 283.15 and 298.15 K using a static method.The equilibrium data obtained have been correlated with the total-pressure method using both the Redlich-Kwong equation of state modified by Soave and the perturbation equation proposed by Gubbins and Twu. From normal probability plots of the residuals in the correlations versus the theoretical residuals in the normal distribution, the applicability of each of these two equations has been tested statistically.Furthermore, the fugacity coefficients calculated from the virial equation have been compared with those obtained from the correlations for the low-pressure regions. 相似文献
49.
A mechanism of heme metabolism by heme oxygenase (HO) is discussed from B3LYP density functional theory calculations. The concerted OH group attack to the alpha-carbon by the iron-hydroperoxo species is investigated using a model with full protoporphyrin IX to confirm our previous conclusion that this species does not have sufficient oxidizing power for heme oxidation (J. Am. Chem. Soc. 2004, 126, 3672). Calculated activation energies and structures of the intermediates and transition state for this process remain unchanged from those for a small model with porphine in the previous study, which shows that the inclusion of the side chain of the porphyrin ring is not essential in describing the OH group transfer. The activation barrier for a direct oxo attack to the alpha-carbon by an iron-oxo model is calculated to be 49.8 kcal/mol, the barrier height of which looks very high for the enzymatic reaction under physiological conditions. This large activation energy is due to a highly bent porphyrin structure in the transition state. However, a bridging water molecule plays an important role in reducing the porphyrin distortion in the transition state, resulting in a remarkable decrease of the activation barrier to 13.9 kcal/mol. A whole-enzyme model with about 4000 atoms is constructed to elucidate functions of the protein environment in this enzymatic reaction using QM/MM calculations. The key water molecule is fixed in the protein environment to ensure the low-barrier and regioselective heme oxidation. A water-assisted oxo mechanism of heme oxidation by heme oxygenase is proposed from these calculational results. 相似文献
50.
Kazunari Shima 《Zeitschrift fur Physik C Particles and Fields》1983,18(1):25-30
From the group theoretical arguments, we find that among allSO(N) supergravitiesN=10 is the minimal supersymmetry group which unifies all fundamental forces of weak, electromagnetic, strong and gravitational interactions. The (super)symmetry is broken throughSO(10)→SU(3)?SU(2)?U(1)→SU(3)?U(1). All observed particles of the low energy physics (three generations of quarks and leptons, γ,Z, W ± and gluons) and graviton can be minimally accomodated with the correctSU(3)?SU(2)?U(1) quantum numbers. Some characteristic predictions, which can be checked in the coming high energy experiments, are briefly discussed. 相似文献