首页 | 本学科首页   官方微博 | 高级检索  
文章检索
  按 检索   检索词:      
出版年份:   被引次数:   他引次数: 提示:输入*表示无穷大
  收费全文   1577篇
  免费   285篇
  国内免费   159篇
化学   988篇
晶体学   9篇
力学   145篇
综合类   30篇
数学   278篇
物理学   571篇
  2024年   1篇
  2023年   40篇
  2022年   45篇
  2021年   41篇
  2020年   80篇
  2019年   61篇
  2018年   41篇
  2017年   50篇
  2016年   70篇
  2015年   77篇
  2014年   85篇
  2013年   109篇
  2012年   146篇
  2011年   142篇
  2010年   106篇
  2009年   99篇
  2008年   99篇
  2007年   83篇
  2006年   96篇
  2005年   49篇
  2004年   59篇
  2003年   42篇
  2002年   36篇
  2001年   23篇
  2000年   39篇
  1999年   28篇
  1998年   33篇
  1997年   29篇
  1996年   26篇
  1995年   22篇
  1994年   16篇
  1993年   21篇
  1992年   25篇
  1991年   12篇
  1990年   16篇
  1989年   14篇
  1988年   4篇
  1987年   7篇
  1986年   11篇
  1985年   13篇
  1984年   9篇
  1983年   8篇
  1982年   2篇
  1981年   3篇
  1980年   1篇
  1979年   2篇
排序方式: 共有2021条查询结果,搜索用时 156 毫秒
91.
92.
The mass of the tritium produced in 6Li(n,α)T reaction was obtained by quantitatively analyzing the byproduct 4He with mass spectrometer. The self-expending seal method was employed to quantitatively prepare the Li–Pb alloy targets in room temperature. They were irradiated for 2 h in two rabbit irradiation channels in Xi’an pulsed reactor and measured after cooling 15 days. A sample purifying unit was set up to get rid of the hydrogen isotopes to remarkably reduce the interference to helium isotopes when measuring. And the sample disposal platform including purifying unit was testified with simulative gas and nature atmosphere. The targets were melted at 700 °C to release most of the 4He atoms which were measured by adding dilution gas 3He. And it was testified that 4He had released completely by repetitiously melting the targets. This approach had solved the problem that the tritium couldn’t be accurately determined by directly analyzing it because of non-complete releasing from lithium alloy.  相似文献   
93.
Yin  Jin  Ouyang  Qing-Feng  Sun  Zhao-Bo  Wu  Feng-Yang  Liu  Qian  Zhang  Xi-Xi  Xu  Ling  Lin  Hao  Zhong  Gan-Ji  Li  Zhong-Ming 《高分子科学》2022,40(6):593-601

Components of co-continuous phase can form an interpenetrating network structure, which has great potential to synergistically improve the mechanical properties of the blends, and to impart the functional blends superior electrical conductivity and permeability. In this work, the effects of shear rates (50–5000 s?1) at different temperatures on the phase morphology, phase size and lamellar crystallites of biodegradable co-continuous polybutylene terephthalate (PBAT)/polybutylene succinate (PBS) blend are quantitatively investigated. The results show that the above features of the PBAT/PBS have a strong dependence on the shear flow and thermal field. The co-continuous phase of the blend is well maintained at 130 °C. Interestingly, this phase structure transforms into a “sea-island” structure at 160 °C, which gradually recovers to a co-continuous phase when the shear rate increases from 1000 s?1 to 5000 s?1. The phase size decreases with the increase of shear rate both at 130 °C and 160 °C due to the refinement and deformation of phase structures caused by strong shear stress. Unexpectedly, a unique phenomenon is observed that the shear-induced lamellar crystallites are oriented perpendicular to shear direction in the range of 500–5000 s?1 at 130 °C, while the orientation of lamellar crystallites at 160 °C is along the shear direction within the whole range of shear rates. The degree of orientation for the PBAT/PBS blend crystals increases first and then decreases at both temperatures above. In addition, the range of shear rate has reached the level in the industrial processing. Therefore, this work has important guiding significance for the regulation of the co-continuous phase structure and the performance for the blend in the practical processing.

  相似文献   
94.
木质素是一种天然芳香族聚合物,约占木质纤维素的30%,是唯一通过裂解C―O醚键和C―C键生产芳香族化学品或液体燃料的可再生芳香族资源。迄今为止,对木质素氢解制备有价值化合物的研究主要集中在相对不稳定的C―O键的裂解上,这限制了木质素氢解的效率。采用水热法和湿浸渍法制备了多功能Pt/NbPWO催化剂。通过破坏碱木质素中的C―O键和C―C键,可以得到产率为18.02%的芳香族单体。该反应不仅可以断裂木质素聚合物中醚键,同时也可以断裂部分关键的C―C键。其氢解机理可能是丰富的Brønsted酸和Lewis酸位点参与了C―C的活化。此外,重点分析载体和Pt物种在Pt/NbPWO催化剂中的协同作用。  相似文献   
95.
Antibiotics, once being released into the environment, become recalcitrant organic pollutants, which pose a potential risk to ecological balance and human health. In this study, a Z-scheme heterojunction of bismuth oxyiodide (BiOI)/exfoliated g-C3N4 (BiOI/ECN hereafter) was synthesized by the combination of thermal exfoliation of g-C3N4 and chemical precipitation of BiOI for efficient photocatalytic degradation of tetracycline in aqueous solutions under visible light irradiation. The optimized BiOI/ECN delivered an outstanding degradation rate at circa 0.0705 min?1, which was 10 times higher than that of the bulk g-C3N4. The photocatalytic degradation efficiency of tetracycline remained almost unchanged in a pH range of 3–11, and the BiOI/ECN displayed an excellent photostability upon recycled usage. The photocatalytic mechanism of tetracycline was ascribed to the main reactive oxidation species of photogenerated holes and superoxide radicals. In addition, the possible degradation pathways of tetracycline were investigated by HPLC-MS to identify intermediates. The toxicity of photocatalytic-generated intermediates of tetracycline was found significantly alleviated according to the calculation of quantitative structure–activity relationship prediction. This work not only provides an attractive photocatalyst for the removal of tetracycline but also opens a new avenue for rational design of Z-scheme heterojunction composites for tetracycline degradation.  相似文献   
96.
Addressing arsenite pollution in groundwater has drawn great attention. It is attractive to pre-oxidize highly mobile As(III) to relatively low-toxic As(V) with a subsequent adsorption separation process. Herein, BiOI anchoring on γ-Fe2O3 is performed to synthesize BiOI/γ-Fe2O3 core–shell nanoparticles for efficient removal of As(III) via a simultaneous photocatalytic oxidization–adsorption process. The physical and chemical structures of BiOI/γ-Fe2O3 are investigated by transmission electron microscopy, Fourier transform infrared spectroscopy, and X-ray diffraction measurements. The photoluminescence and electron spin resonance (ESR) characterization were employed to ascertain the possible reaction mechanism of visible-light-driven photocatalytic oxidation of As(III). Such BiOI/γ-Fe2O3 delivers a superior As(III) removal capability under visible light irradiation with an arsenic removal efficiency of 99.8% within 180 min, higher than those of BiOCl/γ-Fe2O3 (81.7%) and BiOBr/γ-Fe2O3 (98.9%). The optimal BiOI/γ-Fe2O3 (molar ratio of 2:1) is obtained by rationally adjusting the molar ratio of BiOI to γ-Fe2O3. The as-synthesized BiOI/γ-Fe2O3 performs well in a wide pH range of 2–8. Only coexisting PO43? anions have a significant effect on the As(III) removal. The free radical trapping experiment and ESR results demonstrate that the ?O2? and h+ are the main active substances for the photocatalytic oxidation of As(III) on BiOI/γ-Fe2O3. This work not only gives a novel magnetic core–shell nanoparticle photocatalyst for efficient photocatalytic oxidation and adsorption of As(III) but also offers a new strategy to rationally design BiOX for its related practical applications.  相似文献   
97.
Adsorptive separation of C2H6 from C2H4 by adsorbents is an energy-efficient and promising method to boost the polymer grades C2H4 production. However, that C2H6 and C2H4 display very similar physical properties, making their separation extremely challenging. In this work, by regulating the pore environment in a family of chitosan-based carbon materials (C-CTS-1, C-CTS-2, C-CTS-4, and C-CTS-6)- we target ultrahigh C2H6 uptake and C2H6/C2H4 separation, which exceeds most benchmark carbon materials. Explicitly, the C2H6 uptake of C-CTS-2 (166 cm3/g at 100 kPa and 298 K) has the second-highest adsorption capacity among all the porous materials. In addition, C-CTS-2 gives C2H6/C2H4 selectivity of 1.75 toward a 1:15 mixture of C2H6/C2H4. Notably, the adsorption enthalpies for C2H6 in C-CTS-2 are low (21.3 kJ/mol), which will facilitate regeneration in mild conditions. Furthermore, C2H6/C2H4 separation performance was confirmed by binary breakthrough experiments. Under different ethane/ethylene ratios, C-CTS-X extracts a low ethane concentration from an ethane/ethylene mixture and produces high-purity C2H4 in one step. Spectroscopic measurement and diffraction analysis provide critical insight into the adsorption/separation mechanism. The nitrogen functional groups on the surface play a vital role in improving C2H6/C2H4 selectivity, and the adsorption capacities depend on the pore size and micropore volume. Moreover, these robust porous materials exhibit outstanding stability (up to 800 °C) and can be easily prepared on a large scale (kg) at a low cost (~$26 per kg), which is very significant for potential industrial applications.  相似文献   
98.
基于光导微探针的近场/远场可扫描太赫兹光谱技术   总被引:2,自引:0,他引:2       下载免费PDF全文
太赫兹技术已经成为涉及公共安全、军事国防和国民经济等国家核心利益的前沿研究领域.以往太赫兹测量技术中通常以远场测量为主,如常用的太赫兹时域光谱仪.近年来太赫兹近场技术得到了迅猛的发展,特别是基于光导天线的探针技术的发展,为可扫描的太赫兹近场测量提供了可能.本文详细报道了我们近期在可扫描太赫兹近场光谱仪研究中的进展.采用光纤耦合的光导微探针实现了方便灵活的太赫兹近场/远场三维扫描,并同时获得振幅和相位信息.该系统将有可能广泛应用于人工微结构、石墨烯、表面等离子激元、波导传输、近场成像、生物样品检测、芯片检测等研究领域.  相似文献   
99.
Brain asymmetry is a phenomenon well known for handedness and has been studied in motor cortices. However, few quantitative studies on asymmetrical cortical activity in motor areas have been conducted. In this study, we systematically investigated asymmetrical cortical activity in motor areas during sequential finger movement by quantitatively analyzing functional magnetic resonance imaging (fMRI) blood oxygenation level-dependent (BOLD) responses. The norm of BOLD signal percentage of change was introduced to quantitatively measure the BOLD signal intensity change difference between the left and right motor areas. The results of the data collected from six subjects show that the norm of BOLD signal percentage of change in the right motor area is higher than that in the left motor area for two-hand movement (P=.0059) and single-hand movement (P=.0279) with right-handedness. These results from fMRI show the asymmetry of motor areas and may suggest that the left hemisphere motor area comes into being as an adaptation system that needs few neuron cells only to finish any movement task for right-handedness. The activation intensity in the left motor area is reduced with normal right finger movement. The activation intensity in the right motor area is obviously higher than that in the left motor area.  相似文献   
100.
In this work, various Co3O4-ZSM-5 catalysts were prepared by the microwave hydrothermal method (MH-Co3O4@ZSM-5), dynamic hydrothermal method (DH-Co3O4@ZSM-5), and conventional hydrothermal method (CH-Co3O4/ZSM-5). Their catalytic oxidation of dichloromethane (DCM) was analyzed. Detailed characterizations such as X-ray diffractometer (XRD), scanning microscopy (SEM), X-ray photoelectron spectroscopy (XPS), Brunauer–Emmett–Teller (BET), H2 temperature-programmed reduction (H2-TPR), temperature-programmed desorption of O2 (O2-TPD), temperature-programmed desorption of NH3 (NH3-TPD), diffuse reflectance infrared Fourier-transform spectra with NH3 molecules (NH3-DRIFT), and temperature-programmed surface reaction (TPSR) were performed. Results showed that with the assistance of microwave, MH-Co3O4@ZSM-5 formed a uniform core-shell structure, while the other two samples did not. MH-Co3O4@ZSM-5 possessed rich surface adsorbed oxygen species, higher ratio of Co3+/Co2+, strong acidity, high reducibility, and oxygen mobility among the three Co3O4-ZSM-5 catalysts, which was beneficial for the improvement of DCM oxidation. In the oxidation of dichloromethane, MH-Co3O4@ZSM-5 presented the best activity and mineralization, which was consistent with the characterizations results. Meanwhile, according to the TPSR test, HCl or Cl2 removal from the catalyst surface was also promoted in MH-Co3O4@ZSM-5 by their abundant Brønsted acid sites and the promotion of Deacon reaction by Co3O4 or the synergistic effect of Co3O4 and ZSM-5. According to the results of in situ DRIFT studies, a possible reaction pathway of DCM oxidation was proposed over the MH-Co3O4@ZSM-5 catalysts.  相似文献   
设为首页 | 免责声明 | 关于勤云 | 加入收藏

Copyright©北京勤云科技发展有限公司  京ICP备09084417号