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1.
Hydrothermal synthesis using graphene oxide (GO) as a precursor has been used to produce luminescent graphene quantum dots (GQDs). However, such a method usually requires many reagents and multistep pretreatments, while can give rise to GQDs with low quantum yield (QY). Here, we investigated the concentration, the temperature of synthesis, and the pH of the GO solution used in the hydrothermal method through factorial design experiments aiming to optimize the QY of GQDs to reach a better control of their luminescent properties. The best synthesis condition (2 mg/mL, 175 °C, and pH = 8.0) yielded GQDs with a relatively high QY (8.9%) without the need of using laborious steps or dopants. GQDs synthesized under different conditions were characterized to understand the role of each synthesis parameter in the materials' structure and luminescence properties. It was found that the control of the synthesis parameters enables the tailoring of the amount of specific oxygen functionalities onto the surface of the GQDs. By changing the synthesis' conditions, it was possible to prioritize the production of GQDs with more hydroxyl or carboxyl groups, which influence their luminescent properties. The as-developed GQDs with tailored composition were used as luminescent probes to detect Fe3+. The lowest limit of detection (0.136 μM) was achieved using GQDs with higher amounts of carboxylic groups, while wider linear range was obtained by GQDs with superior QY. Thus, our findings contribute to rationally produce GQDs with tailored properties for varied applications by simply adjusting the synthesis conditions and suggest a pathway to understand the mechanism of detection of GQDs-based optical sensors.  相似文献   
2.
针对考虑几何和材料非线性的石英晶体板厚度剪切振动和弯曲振动的方程组,利用扩展伽辽金法对该方程组进行转化和求解,分别获得了强烈耦合的厚度剪切振动模态和弯曲振动模态的频率响应关系,绘制了不同振幅比和不同驱动电压影响下的频率响应曲线图。数值计算结果表明可以选取石英晶片的最佳长厚比尺寸来避免两种模态的强烈耦合。驱动电压的变化将引起石英晶体谐振器厚度剪切振动频率的明显改变,必须将振动频率的漂移值控制在常用压电声波器件的允许值之内。扩展伽辽金法对石英晶体板非线性振动方程组的求解为非线性有限元分析和偏场效应分析奠定了基础。  相似文献   
3.
We consider parametric optimization problems from an algebraic viewpoint. The idea is to find all of the critical points of an objective function thereby determining a global optimum. For generic parameters (data) in the objective function the number of critical points remains constant. This number is known as the algebraic degree of an optimization problem. In this article, we go further by considering the inverse problem of finding parameters of the objective function so it gives rise to critical points exhibiting a special structure. For example if the critical point is in the singular locus, has some symmetry, or satisfies some other algebraic property. Our main result is a theorem describing such parameters.  相似文献   
4.
In the present paper,we study the restricted inexact Newton-type method for solving the generalized equation 0∈f(x)+F(x),where X and Y are Banach spaces,f:X→Y is a Frechet differentiable function and F:X■Y is a set-valued mapping with closed graph.We establish the convergence criteria of the restricted inexact Newton-type method,which guarantees the existence of any sequence generated by this method and show this generated sequence is convergent linearly and quadratically according to the particular assumptions on the Frechet derivative of f.Indeed,we obtain semilocal and local convergence results of restricted inexact Newton-type method for solving the above generalized equation when the Frechet derivative of f is continuous and Lipschitz continuous as well as f+F is metrically regular.An application of this method to variational inequality is given.In addition,a numerical experiment is given which illustrates the theoretical result.  相似文献   
5.
The effect of ultrasound on the kinetics of anti-solvent crystallization of sucrose was studied. The influence of temperature, stirring rate, supersaturation and ultrasonic power on the anti-solvent crystallization of sucrose was investigated. The relationship between infrared spectral characteristic band of sucrose and supersaturation was determined with an online reaction analyzer. The crystal size distribution of sucrose was detected by a laser particle-size analyzer. Ultrasound accelerated the crystallization process, and had no impact on the crystal shape. Abegg, Stevens and Larson model was fitted to the experimental data, and the results were the following: At 298.15 K, the average size of crystals was 133.8 μm and nucleation rate was 4.87 × 109 m−3·s−1 without ultrasound. In an ultrasonic field, the average size was 80.5 μm, and nucleation rate was 1.18 × 1011 m−3·s−1. Ultrasound significantly reduced the average size of crystals and improved the nucleation rate. It was observed that the crystal size decreased with the increase of stirring rate in silent environment. When the stirring rate increased from 250 to 400 rpm, the average size decreased from 173.0 to 132.9 μm. However, the stirring rate had no significant impact on the crystal size in the ultrasonic field. In addition, the activation energy of anti-solvent crystallization of sucrose was decreased, and the kinetic constant of nucleation rate was increased due to the effect of ultrasound. In the ultrasonic field, the activation energy was reduced from 20422.5 to 790.5 J·mol−1, and the kinetic constant was increased from 9.76 × 102 to 8.38 × 108.  相似文献   
6.
氮和磷是水环境生物生长和繁殖必须的营养成分,影响水体初级生产力的水平,且水体富营养化水平与氮磷形态密切相关,随着水体环境的改变,沉积物会向水体释放氮磷,造成二次污染。同时,对外源氮磷污染来源的贡献进行定量识别,可有效管理和控制水体氮磷污染负荷。毗河和石亭江是沱江的重要支流,影响着长江母亲河的水质。采用钼锑抗分光光度法和连续提取法研究在枯水期和丰水期毗河和石亭江水体和表层沉积物中总氮(TN)、总磷(TP)及各形态氮磷的分布特性,对比不同土地利用类型河流氮磷行为特性及释放风险,并采用Multiple Linear Regression of the Absolute Principal Component Scores(APCS-MLR)受体模型进行氮磷污染源的识别和量化。研究结果表明:① 研究区水体和表层沉积物中氮磷均处于不同程度的污染水平,水体枯水期TP的主要贡献者是颗粒态无机磷(PIP)和颗粒态有机磷(POP),而丰水期却是颗粒态无机磷(PIP)和溶解态无机磷(DIP),两水期水体中TN的主要贡献者是硝态氮(NO-3-N)和有机氮(ON)。而在表层沉积物中,TP的主要贡献者是钙结合态磷(HCl-P),TN的主要贡献者是酸解态氮(HN)。在枯水期和丰水期,毗河表层沉积物生物有效磷(BAP)占TP的平均值(19.7%和23.0%)比石亭江的平均值(11.0%和12.5%)占比更高,具有较高的磷释放风险。研究发现,枯水期氮磷污染程度高于丰水期,而且石亭江的氮磷污染程度高于毗河。②APCS-MLR模型在毗河提取了城镇生活污水、生活垃圾堆积产生的渗滤液、动植物残体分解和养殖业废水4个污染源因子,其中城镇生活污水对毗河氮磷污染的贡献最大(枯水期50.9%,丰水期54.8%),而在石亭江提取了工业生产中产生的废水等、动植物残体的降解、农业废弃物的风化、农田排水渠的农业废水和农药化肥的不合理施用5个污染源因子,其中工业生产中产生的废水等对石亭江氮磷污染的贡献最大(枯水期58.7%,丰水期55.8%)。因此,当地相关部门应加强对高贡献污染源的管控,从而降低流域氮磷污染负荷。  相似文献   
7.
采用水热-煅烧法制备Cd2SnO4,之后通过超声混合法得到一系列MoS2/Cd2SnO4复合材料。采用X射线衍射、扫描电子显微镜、X射线光电子能谱对Cd2SnO4和一系列MoS2/Cd2SnO4复合材料进行结构和形貌的表征。研究了MoS2掺杂量对于MoS2/Cd2SnO4复合材料的气敏性能影响。实验结果表明,当MoS2与Cd2SnO4的质量比为2.5%,MoS2/Cd2SnO4复合材料制备的气敏元件在170 ℃时对浓度为100 μL·L-1的甲醛气体的灵敏度为40.0,最低检测限为0.1 μL·L-1。  相似文献   
8.
The reaction of N2 with trinuclear niobium and tungsten sulfide clusters Nb3Sn and W3Sn (n=0–3) was systematically studied by density functional theory calculations with TPSS functional and Def2-TZVP basis sets. Dissociations of N−N bonds on these clusters are all thermodynamically allowed but with different reactivity in kinetics. The reactivity of Nb3Sn is generally higher than that of W3Sn. In the favorite reaction pathways, the adsorbed N2 changes the adsorption sites from one metal atom to the bridge site of two metal atoms, then on the hollow site of three metal atoms, and at that place, the N−N bond dissociates. As the number of ligand S atoms increases, the reactivity of Nb3Sn decreases because of the hindering effect of S atoms, while W3S and W3S2 have the highest reactivity among four W3Sn clusters. The Mayer bond order, bond length, vibrational frequency, and electronic charges of the adsorbed N2 are analyzed along the reaction pathways to show the activation process of the N−N bond in reactions. The charge transfer from the clusters to the N2 antibonding orbitals plays an essential role in N−N bond activation, which is more significant in Nb3Sn than in W3Sn, leading to the higher reactivity of Nb3Sn. The reaction mechanisms found in this work may provide important theoretical guidance for the further rational design of related catalytic systems for nitrogen reduction reactions (NRR).  相似文献   
9.
A detailed study of the geometry, aromatic character, electronic and magnetic properties for a series of positively charged N-doped polycyclic aromatic hydrocarbons (PAHs) was performed. Magnetic properties of the examined molecules were analyzed by means of the magnetically induced current density calculated using the diamagnetic-zero version of the continuous transformation of origin of current density (CTOCD-DZ) method. The comparative study of the local aromaticity of the studied molecules was performed using several different indices: energy effect (ef), harmonic oscillator model of aromaticity (HOMA) index, six centre delocalization index (SCI) and nucleus independent chemical shifts (NICS). The presence of N-atoms in the inner rings was found to cause a planarity distortion in the studied N-doped systems. The geometric changes and charged nature of the studied N-doped systems do not significantly influence the current density and the local aromaticity distribution in comparison with the corresponding parent benzenoid hydrocarbons. The present study demonstrates how quantum chemical calculations can be used for rational design of novel PAHs and for fine tuning of their properties.  相似文献   
10.
Dehydrogenation of an organic compound is the first and the most fundamental elementary reaction in many organic reactions. In ethanol oxidation reaction (EOR) to form CO2, there are a total of 46 pathways in C2HxO (x=1–6) species leading to the removal of all six hydrogen atoms in five C−H bonds and one O−H bond. To investigate the degree of dehydrogenation in EOR under operando conditions, we performed density function theory (DFT) calculations to study 28 dehydrogenation steps of C2HxO on Ir(100). An activation energy surface was then constructed and compared with that of the C−C bond cleavages to understand the importance of the degree of dehydrogenation in EOR. The results show that there are likely 28 dehydrogenations in EOR under fuel cell temperatures and the last two hydrogens in C2H2O are less likely cleaved. On the other hand, deep dehydrogenation including 45 dehydrogenations can occur under ethanol steam reforming conditions.  相似文献   
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