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   293篇
  免费   45篇
  国内免费   31篇
化学   229篇
晶体学   2篇
力学   11篇
综合类   2篇
数学   31篇
物理学   94篇
  2024年   3篇
  2023年   7篇
  2022年   22篇
  2021年   18篇
  2020年   25篇
  2019年   19篇
  2018年   18篇
  2017年   8篇
  2016年   22篇
  2015年   17篇
  2014年   25篇
  2013年   17篇
  2012年   34篇
  2011年   29篇
  2010年   14篇
  2009年   20篇
  2008年   11篇
  2007年   12篇
  2006年   9篇
  2005年   7篇
  2004年   5篇
  2003年   4篇
  2002年   2篇
  2001年   4篇
  2000年   3篇
  1997年   1篇
  1996年   1篇
  1994年   2篇
  1993年   1篇
  1992年   1篇
  1991年   3篇
  1990年   1篇
  1986年   2篇
  1984年   2篇
排序方式: 共有369条查询结果,搜索用时 15 毫秒
361.
Effective fault-diagnosis strategies have been the focus of research on multi-agent systems (MASs). In this paper, the belief rule base (BRB)-based distributed fault-diagnosis problem for MASs is investigated, and a topology-switching strategy is developed to increase the reliability of fault-diagnosis model. Firstly, a BRB-based distributed fault-diagnosis model is constructed for the MAS with multiple faults, then expert knowledge is used to judge whether the agent is faulty. Then, considering that the system may be influenced by the fault or some other factors and thus leading to a decrease in the accuracy of the fault-diagnosis results, a topology-switching strategy based on the average distance of the output diagnosis accuracy is proposed to update the topology of the agent so that the fault-diagnosis results can be more reliable. Note that the topology-switching threshold is designed based on the average distance between the accuracy of the fault diagnosis of each agent. The method proposed in this paper can solve the problem when the fault-diagnosis accuracy of the model is affected by some common factors and thus decreases, and can improve the reliability of the fault-diagnosis model very well. Finally, the effectiveness of the BRB-based distributed fault-diagnosis model and the proposed topology-switching strategy to improve the fault-diagnosis accuracy is verified by simulation examples.  相似文献   
362.
通过氢气原位程序升温还原法制备了一系列不同Ce/Ni摩尔比的CePO4-Ni3P及Ni3P催化剂,考察了其在苯酚催化转移加氢反应的催化性能.研究了Ce/Ni摩尔比、供氢溶剂、反应温度和反应时间对催化剂性能的影响,并初步考察了苯酚转移加氢的反应动力学.研究结果表明,CePO4的加入能显著提升体相Ni3P催化苯酚转移加氢的转化率,且Ce/Ni摩尔比为0. 2时促进作用最显著;在所考察的供氢溶剂中异丙醇展现出最好的性能;使用Ce PO4(0. 2)-Ni3P作为反应催化剂,异丙醇作为供氢溶剂,220℃下反应6 h,苯酚转化率和环己醇选择性分别可达93. 1%和92. 0%.  相似文献   
363.
制备了一种含有联吡啶位点的共价有机骨架(COF)材料TpBpy,并通过配体上的联吡啶位点固载铜盐实现了功能化,得到的Cu@TpBpy具有大量的不饱和铜配位位点和高表面积,可用作苯硼酸与咪唑的Chan-Lam偶联反应的多相催化剂.通过优化溶剂、铜源、碱及反应时间等反应条件,发现使用质子极性溶剂MeOH时的反应产率最高,而Cu(OAc)2@Tp Bpy是效果最佳的催化剂,可溶性有机碱三乙胺(TEA)的促进效果最好.Cu(OAc)2@TpBpy在碱TEA的促进下于70℃催化咪唑与苯硼酸反应4 h后,得到目标产物1-苯基咪唑的最大产率为66%.在最优反应条件下进行了底物拓展,结果表明,取代基的位阻效应对催化体系影响显著,其中对位取代基的4-氯苯硼酸的产率最高(62%).  相似文献   
364.
365.
Developing a novel tool capable of real-time monitoring and simultaneously quantifying of both intra/extracellular chemical signals across the large-scale brain is the key bottleneck for understanding the interactions between the molecules inside and outside neurons. Here we built up a high-density intra/extracellular optophysiology platform, together with developing two probes for specific recognition of L-cysteine (Cys) and dopamine (DA), for simultaneously quantifying of both intracellular Cys and extracellular DA with high selectivity and accuracy across the brain of freely moving animals, as well as recording electrical signals. Using this powerful tool, it was found that intracellular Cys regulated extracellular DA through inducing the expression of tyrosine hydroxylase in the depressed mice brain. We also established the functional networks of Cys and DA across 32 brain regions in freely moving animals. More importantly, it was discovered that depression reduced the correlations between adjacent brain regions, which was recovered by the treatment of N-acetyl-l-cysteine.  相似文献   
366.
Activation of nitromethane to endow new reactivity is an interesting and meaningful but also challenging topic. Herein, we report an electrochemical activation of nitromethane to serve as both the heterocyclic skeleton and oxime sources for the construction of isoxazoline aldoximes. The isoxazoline aldoximes that are prepared by four steps with the reported strategy are synthesized in a single step from low-cost and readily available nitromethane and olefins with moderate to excellent yields under our electrochemical conditions. The reaction also takes advantage of high atom-economy and E-selectivity. Moreover, the mechanism is studied by control experiments, a kinetic isotope effect (KIE) study, cyclic voltammogram (CV) experiments, and density functional theory (DFT) calculations. The mechanistic results reveal that nitromethane may be activated under electrochemical conditions to deliver a 1,2,5-oxadiazole 2-oxide intermediate, which undergoes [3+2] cycloaddition with olefins to yield isoxazoline aldoximes.  相似文献   
367.
In conventional luminol electrochemiluminescence (ECL) systems, hydrogen peroxide and dissolved oxygen are employed as typical co-reactants to produce reactive oxygen species (ROS) for efficient ECL emission. However, the self-decomposition of hydrogen peroxide and limited solubility of oxygen in water inevitably restrict the detection accuracy and luminous efficiency of luminol ECL system. Inspired by ROS-mediated ECL mechanism, for the first time, we used cobalt-iron layered double hydroxide as co-reaction accelerator to efficiently activate water to generate ROS for enhancing luminol emission. Experimental investigations verify the formation of hydroxyl and superoxide radicals in the process of electrochemical water oxidation, which subsequently react with luminol anion radicals to trigger strong ECL signals. Finally, the detection of alkaline phosphatase has been successfully achieved with impressive sensitivity and reproducibility for practical sample analysis.  相似文献   
368.
设计、合成了2个配合物:{[Co2(pddb)2μ2-H2O)(H2O)2]·2DMA·5H2O}n1)和{[Ni2(pddb)2μ2-H2O)(H2O)2]·2DMA·5H2O}n2)(H2pddb=3,3''-(吡啶-3,5)二苯甲酸,DMA=N,N-二甲基乙酰胺),并通过红外光谱(IR),元素分析,热重分析(TG)和单晶X射线衍射确定它们的结构。结构分析表明12是异质同构的,其空间构型可简化成(3,6)连接的拓扑结构,其符号为(42·6)·(44·62·88·10)。进一步研究了配合物12的固体紫外、磁性及其催化性能。研究表明12中的中心金属离子之间存在反铁磁耦合作用,并且1可以作为C-H活化的高效非均相催化剂。  相似文献   
369.
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