首页 | 官方网站   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   5301篇
  免费   997篇
  国内免费   528篇
数理化   6826篇
  2024年   23篇
  2023年   123篇
  2022年   198篇
  2021年   203篇
  2020年   204篇
  2019年   196篇
  2018年   193篇
  2017年   143篇
  2016年   258篇
  2015年   266篇
  2014年   266篇
  2013年   346篇
  2012年   499篇
  2011年   551篇
  2010年   327篇
  2009年   334篇
  2008年   350篇
  2007年   291篇
  2006年   265篇
  2005年   210篇
  2004年   185篇
  2003年   127篇
  2002年   146篇
  2001年   112篇
  2000年   121篇
  1999年   109篇
  1998年   94篇
  1997年   107篇
  1996年   86篇
  1995年   79篇
  1994年   63篇
  1993年   72篇
  1992年   42篇
  1991年   63篇
  1990年   42篇
  1989年   36篇
  1988年   15篇
  1987年   14篇
  1986年   18篇
  1985年   15篇
  1984年   11篇
  1983年   11篇
  1982年   7篇
  1981年   2篇
  1979年   1篇
  1976年   1篇
  1971年   1篇
排序方式: 共有6826条查询结果,搜索用时 15 毫秒
81.
The lack of suitable lightweight current collectors is one of the primary obstacles preventing the energy density of aqueous lithium-ion batteries (ALIBs) from becoming competitive. Using silver nanowire (AgNW) films as current collectors and a molecular crowding electrolyte, we herein report the fabrication of ALIBs with relatively good energy densities. In the 2 m LiTFSI–94% PEG–6% H2O solution, the AgNW films with a sheet resistance of less than 1.0 ohm/square exhibited an electrochemical stability window as broad as 3.8 V. The LiMn2O4//Li4Ti5O12 ALIBs using AgNW films as the current collectors demonstrated an initial energy density of 70 Wh/kg weighed by the total mass of the cathode and anode, which retained 89.1% after 50 cycles.  相似文献   
82.
Determining the different surfaces of oxide nanocrystals is key in developing structure–property relations. In many cases, only surface geometry is considered while ignoring the influence of surroundings, such as ubiquitous water on the surface. Here we apply 17O solid-state NMR spectroscopy to explore the facet differences of morphology-controlled ceria nanocrystals considering both geometry and water adsorption. Tri-coordinated oxygen ions at the 1st layer of ceria (111), (110), and (100) facets exhibit distinct 17O NMR shifts at dry surfaces while these 17O NMR parameters vary in the presence of water, indicating its non-negligible effects on the oxide surface. Thus, the interaction between water and oxide surfaces and its impact on the chemical environment should be considered in future studies, and solid-state NMR spectroscopy is a sensitive approach for obtaining such information. The work provides new insights into elucidating the surface chemistry of oxide nanomaterials.

Both atomic geometry and the influence of surroundings (e.g., exogenously coordinated water) are key issues for determining the chemical environment of oxide surfaces, whereas the latter is usually ignored and should be considered in future studies.  相似文献   
83.
Inducing the surface enrichment of active noble metal can not only help to stabilize the catalyst but also modify the catalytic performance of the catalyst through electronic and geometric effects. Herein, we report the in situ surface enrichment of Ir on IrRu alloy during the oxygen evolution reaction (OER). The surface enrichment of Ir was probed by ex situ high-resolution transmission electron microscopy (HRTEM), in situ X-ray absorption spectroscopy (XAS), and electrochemical Cu stripping, leading to complementary characterizations of the dynamic reconstruction of the IrRu alloy during OER. Guided by the density functional theory (DFT), an IrRu alloy with low Ir content (20 wt%) was constructed, which displayed a low overpotential of only 230 mV to deliver an OER current density of 10 mA cm−2 in 0.1 M HClO4 solution and maintained stable performance for over 20 h. To investigate the practical application potential, a proton exchange membrane (PEM) water electrolyzer using the IrRu alloy as the anode catalyst was assembled, which required a low cell voltage of only 1.48 V to generate a current density of 1 A cm−2.

Inducing the surface enrichment of active noble metal can not only help to stabilize the catalyst but also modify the catalytic performance of the catalyst through electronic and geometric effects.  相似文献   
84.
The determination of directed control paths in complex networks is important because control paths indicate the structure of the propagation of control signals through edges. A challenging problem is to identify them in complex networked systems characterized by different types of interactions that form multilayer networks. In this study, we describe a graph pattern called the conserved control path, which allows us to model a common control structure among different types of relations. We present a practical conserved control path detection method (CoPath), which is based on a maximum-weighted matching, to determine the paths that play the most consistent roles in controlling signal transmission in multilayer networks. As a pragmatic application, we demonstrate that the control paths detected in a multilayered pan-cancer network are statistically more consistent. Additionally, they lead to the effective identification of drug targets, thereby demonstrating their power in predicting key pathways that influence multiple cancers.  相似文献   
85.
PtCu single-atom alloys (SAAs) open an extensive prospect for heterogeneous catalysis. However, as the host of SAAs, Cu suffers from severe sintering at elevated temperature, resulting in poor stability of catalysts. This paper describes the suppression of the agglomeration of Cu nanoparticles under high temperature conditions using copper phyllosilicate (CuSiO3) as the support of PtCu SAAs. Based on quasi in situ XPS, in situ CO-DRIFTS, in situ Raman spectroscopy and in situ XRD, we demonstrated that the interfacial Cu+–O–Si formed upon reduction at 680 °C serves as the adhesive between Cu nanoparticles and the silicon dioxide matrix, strengthening the metal–support interaction. Consequently, the resistance to sintering of PtCu SAAs was improved, leading to high catalytic stability during propane dehydrogenation without sacrificing conversion and selectivity. The optimized PtCu SAA catalyst achieved more than 42% propane conversion and 93% propylene selectivity at 580 °C for at least 30 hours. It paves a way for the design and development of highly active supported single-atom alloy catalysts with excellent thermal stability.

This paper describes PtCu single-atom alloys supported on copper phyllosilicate via Cu+–O–Si. The catalyst exhibits sintering resistance in propane dehydrogenation reaction without sacrificing activity and selectivity.  相似文献   
86.
磁流变弹性体(magnetorheological elastomer,MRE)因其独特的场相关性能在工程应用领域引起了广泛关注.论文介绍了MRE的最新发展,重点介绍导电性MRE在材料设计、力学行为和实际应用等方面的研究现状.论文从高性能导电性MRE的研制开始,讨论了材料与结构设计中涉及的关键问题;介绍了导电性MRE材料在磁场作用下的磁、力、电学行为的耦合作用机理和相关物理模型;之后对导电性MRE器件的研究现状进行了总结;最后展望了导电性MRE的发展潜力和面临的挑战.  相似文献   
87.
龚敏  文斌  王华 《爆炸与冲击》2015,35(4):576-584

为了提高掘进进尺,以川煤集团绿水洞矿掘进工程为背景,利用动力有限元程序LS-DYNA3D进行掏槽参数优化研究。结合井下现场实验,分析岩巷掏槽爆破不同参数动态应力、破碎范围的变化以及井下实际爆破效果。掏槽中心孔底向孔口平均有效应力峰值在有中心眼爆破较无中心眼爆破时增加了40%以上,中心眼爆破对槽腔底部的形成起主要作用。在其他条件相同的情况下单孔载荷从1.2 kg提高到1.8 kg,掏槽区中心眼底到孔口平均应力只增加20%,并且破碎范围的增加较少,实际进尺增加小于10%。现场掘进实验表明:在常规爆破载荷下,有中心眼比无中心眼爆破深度提高31%~65%,掏槽角小于78°时,随掏槽角度增加爆破进尺下降较平缓; 但掏槽角增至82°左右, 随掏槽角度增加爆破进尺下降明显。

  相似文献   
88.
Different from the conventional piezochromic materials with a mono-redshift of single emission, our well-designed molecule demonstrates a sensitive turn-on and color-tunable piezochromic luminescence in response to the hydrostatic pressure. The molecule PXZ-W-SOF possesses dual-emission and pressure-induced bidirectional shifting characteristics. On the basis of in-depth experimental studies, on one hand, it is confirmed that the origin of the dual-emission behavior is the intramolecular charge transfer, namely thermally activated delayed fluorescence (TADF), and the intermolecular excimer; on the other hand, the emission of the excimer exhibits three-step variations with increasing pressure, which is mainly attributed to the molecular structure and its crystal packing state. The remarkable color change of PXZ-W-SOF from sky-blue to green to deep-blue during the whole process of boosting and releasing pressure is a result of intramolecular and intermolecular energy-transfer interactions. The PXZ-W-SOF molecular model is an extremely rare example of highly sensitive fluorescence tuning driven by TADF and excimer conversion under mechanical stimulation, thus providing a novel mechanism for the field of piezochromism. The unique molecular design also offers a new idea for rare deep-blue and ultraviolet TADF materials.

A high-contrast luminescent material exhibits dual-emission and pressure-induced bidirectional shifting, originating from the cooperative effects of TADF and excimers. It provides a novel mechanism for the piezochromic behavior.  相似文献   
89.
Macroscopic regulation of chiral supramolecular nanostructures in liquid-crystalline block copolymers is of great significance in photonics and nanotechnology. Although fabricating helical phase structures via chiral doping and microphase separation has been widely reported, the chiral memory and self-recovery capacity of asymmetric phase structures are the major challenge and still deeply rely on the presence of chiral additives. Herein, we demonstrate the first controllable chiral microphase separation in an achiral amphiphilic block copolymer consisting of poly(ethylene oxide) and azobenzene (Azo) groups. Chirality can be transferred to the fabricated helical nanostructures by doping with chiral additives (tartaric acid, TA). After the removal of the chiral additives and then performing cross-linking, the formed helical nanostructures will completely dispense with the chiral source. The supramolecular chirality and the micron-scale phase structure can be maintained under UV irradiation and heating-cooling treatment, enabling a reversible “on–off” chiroptical switch feature. This work is expected to avoid the tedious synthesis and expensive raw materials and shows a great application prospect in chiral separation and so on.

A chirality-storing copolymer MPS structure will overcome the external chiral source dependence and avoid tedious synthesis and expensive raw materials.  相似文献   
90.
Sophora japonica L. (SJL) and Robinia pseudoacacia L. (RPL) are widely cultivated in China. However, the utilization of their main by-products are limited due to a lack of comprehensive nutritional attributes. Herein, the proximate composition, mineral elements, fatty acids, amino acids, monosaccharides, and phenolics were analyzed to investigate the nutritional attributes of SJL and RPL. Dietary fiber was the main ingredient in SJL and RPL, followed by protein and lipids. The content of Fe in SJL and RPL was highest, especially in flowers of SJL, reaching about 1179.51 mg/kg. The total unsaturated fatty acids accounted for 89.67% of the bud of SJL. Meanwhile, the essential amino acids contents of the flower and bud of SJL and RPL accounted for 35.95–40.59% of total amino acids. The flower of SJL (373.75 mg/g) exhibited the most abundant monosaccharides. Meanwhile, the total phenolics and flavonoid contents in the buds of SJL and RPL were significantly higher than that of the flower, implying the buds possessed better biological activity. Moreover, the bud of SJL possessed the most abundant phenolics. The results provided a reference for the development of functional food derived from SJL and RPL.  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-23

京公网安备 11010802026262号