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   15931篇
  免费   2897篇
  国内免费   2051篇
化学   11545篇
晶体学   204篇
力学   998篇
综合类   131篇
数学   1618篇
物理学   6383篇
  2024年   69篇
  2023年   358篇
  2022年   693篇
  2021年   666篇
  2020年   752篇
  2019年   782篇
  2018年   658篇
  2017年   615篇
  2016年   848篇
  2015年   911篇
  2014年   1007篇
  2013年   1244篇
  2012年   1517篇
  2011年   1461篇
  2010年   981篇
  2009年   1062篇
  2008年   1123篇
  2007年   940篇
  2006年   876篇
  2005年   726篇
  2004年   542篇
  2003年   405篇
  2002年   367篇
  2001年   314篇
  2000年   247篇
  1999年   257篇
  1998年   196篇
  1997年   193篇
  1996年   158篇
  1995年   153篇
  1994年   115篇
  1993年   120篇
  1992年   97篇
  1991年   84篇
  1990年   64篇
  1989年   42篇
  1988年   43篇
  1987年   34篇
  1986年   30篇
  1985年   31篇
  1984年   16篇
  1983年   20篇
  1982年   6篇
  1981年   9篇
  1980年   6篇
  1979年   8篇
  1977年   4篇
  1975年   5篇
  1965年   4篇
  1957年   3篇
排序方式: 共有10000条查询结果,搜索用时 15 毫秒
971.
在pH3.0的克拉克-鲁布斯缓冲溶液中,铂(Ⅳ)以PtBr5^2-·2CTMAB+的形式从含有0.59mol·L^-1硝酸钠、5.0×10^-3mol·L^-1溴化钾及3.0×10^-1mol·L^-1十六烷基三甲基溴化铵(CTMAB)的试液中定量浮选分离。此方法中浮选分离时试液的总体积定为10mL,其中合0.1mol·L^-1溴化钾溶液0.5mL,0.01mol·L^-1CTMAB溶液3mL及硝酸钠0.5g。试验结果表明:100/lg铂(Ⅳ)有效地与多达1.0mg的铬(Ⅲ)、锰(Ⅱ)、铝(Ⅲ)、镍(Ⅱ)、镓(Ⅲ)、铁(Ⅱ)及锌(Ⅱ)分离,铂(Ⅳ)的浮选率迭100%。此方法应用于已知含铂0.102%(质量分数)的Ni—Pt/Al2O3催化剂的分析,测得铂量的平均值为0.099%,测定值的相对标准偏差(n=7)为2.2%。  相似文献   
972.
Microbial fuel cell (MFC) technology is a novel electricity generation process catalyzed by microorganisms. Much progress is made in the design and construction of MFCs, however the diversity of the electrochemically active microorganisms and the electricity generation mechanisms remain a black box. As sun is a predominantly unused energy resource, here we present a highly enriched phototrophic consortium that can produce electricity in an “H” typed MFC at a high power density (2650 mW m−2, normalized to membrane area) in light, which was eightfold of that produced by non-enriched consortium in the same reactor. Light–dark shift experiments showed that light contributed to the electricity generation. A microbial excreted mediator assisted the electron transfer to the electrode. During the experiment, the accumulation of the mediator over time enhanced the electron transfer rate. The excitation–emission matrix fluorescence spectroscopy results indicated indole group containing compound representing the dominant mediator component.  相似文献   
973.
Graphene nanosheets (GNSs) were prepared from artificial graphite by oxidation, rapid expansion and ultrasonic treatment. The morphology, structure and electrochemical performance of GNSs as anode material for lithium-ion batteries were systematically investigated by high-resolution transmission electron microscope, scanning electron microscope, X-ray diffraction, Fourier transform infrared spectroscopy and a variety of electrochemical testing techniques. It was found that GNSs exhibited a relatively high reversible capacity of 672 mA h/g and fine cycle performance. The exchange current density of GNSs increased with the growth of cycle numbers exhibiting the peculiar electrochemical performance.  相似文献   
974.
“合理”QSAR模型是指在了解配体与受体相互作用模式的前提下建立定量构效关系, 这样避开了传统做法仅仅依靠样本集分子自身信息来构建预测模型的诸多弊端. 本文将此思想应用于肽/蛋白质亲和活性的研究当中, 借助于遗传算法作为虚拟受体结合靶点及相互作用模式的筛选手段得到了一种新的建模技术: 肽/蛋白质结合模式遗传虚拟筛选(genetic virtual screening of combinative mode for peptide/protein, GVSC). 该法成功解决了“合理”QSAR研究中的难题, 即大多数情况下受体结构未知而难以了解配基与之发生的结合方式. 分别使用58个血管紧张素转化酶, 18个Camel抗体蛋白cAb-lys3双位点突变残基对GVSC加以检验, 其结果表明GVSC能够较好地阐明配基与受体之间的作用机理, 并能得到优于传统方法的QSAR模型.  相似文献   
975.
为减少多硫化锂(LIPs)“穿梭效应”及锂枝晶对锂硫电池的影响,采用刮涂法制备中空碳材料修饰隔膜。接触角测试表明修饰隔膜对LIPs具有更强的吸引力,其对LIPs“穿梭”的有效抑制也可以通过渗透性实验进一步得到印证。在隔膜的正极对称电池测试中,电流响应显示中空碳材料的催化使LIPs快速转化为Li2S。通过隔膜的负极对称电池测试发现修饰隔膜呈现出更稳定的电压-时间曲线。为证明隔膜修饰对锂硫电池性能改进的效果,分别采用聚丙烯(PP)隔膜、单面改性和双面改性的PP隔膜组装成纽扣电池并进行电化学测试,其中电极材料的硫负载量为1.8~2.0 mg·cm-2。GITT(恒电流间歇滴定法)测试和锂离子扩散系数计算表明,改性隔膜的离子传输更快且阻抗较小。通过分析第1、5、10、50及100次的充放电循环阻抗谱图发现,中空碳材料的多通道能够为锂离子的传输提供更多的通道,因此能够使锂离子具有更加稳定的扩散行为。在电流密度为0.2C时,由双面改性隔膜组装的锂硫电池在首次充放电时有1 035 mAh·g-1的可逆比容量,700圈后仍有500 mAh·g-1的高比容量,并在高硫负载时表现出500 mAh·g-1的可逆比容量。双面修饰隔膜赋予了锂硫电池优异的电化学性能,这是由于中空碳材料的修饰加速了LIPs的转化和吸附,有效缓解了LIPs的穿梭效应,且对锂枝晶有很好的抑制作用,提高了锂硫电池的安全性。  相似文献   
976.
Periodontitis is a chronic inflammatory disease of tooth support tissues leading to progressive destruction of periodontal soft tissues as well as alveolar bone, and can be treated with anti-inflammatory and bone-protective agents to prevent disease progression. Caffeic acid phenethyl ester (CAPE) is a natural polyphenolic compound with anti-inflammation, anti-oxidation and bone tissue repair efficacy. In this work, we synthesized a thermosensitive hydrogel matrix of acetylated carboxymethyl chitosan (A-CC), and firstly applied for periodontal local drug delivery. The biocompatible CAPE-loaded A-CC hydrogel (CAPE-A-CC) has the advantages of forming a drug depot in situ, sustained release and precisely improving the drug concentration in the lesion sites compared with traditional systemic administration. In addition, CAPE-A-CC could significantly inhibit the expression of inflammatory cytokines of TNF-α, IL-1β, IL-6, and IL-17 in macrophages, and increased the expression of alkaline phosphatase (ALP) in human periodontal ligament stem cells (hPDLSC) related to osteogenesis. This study develops a novel in situ thermosensitive hydrogel delivery system to improve the therapeutic potential of natural active ingredient for periodontitis therapy.  相似文献   
977.
In this study, a pair of chiral copper(I) cluster-assembled materials (R/S- 2 ) was prepared, exhibiting unique photo-response characteristics with a concentration-wavelength correlation property in DMSO solution. By the combination of R/S- 2 with a polymethyl methacrylate (PMMA) matrix, the first photo-activated circularly polarized luminescence (CPL) film was developed, the CPL signal (glum=9×10−3) of which could be induced by UV light irradiation. Moreover, the film exhibited a reversible photo-response and extremely good fatigue resistance. Mechanism study revealed that the photo-response properties of the R/S- 2 solution and film are attributed to the aggregation-induced emission (AIE) characteristics of R/S- 2 and a photo-induced deoxygenation process. This study enriches the types of luminescent cluster-assembled molecules and provides a new strategy for the construction of metal cluster-based stimuli-responsive composite materials.  相似文献   
978.
Shape-changing polymeric materials have gained significant attention in the field of bioinspired soft robotics. However, challenges remain in versatilizing the shape-morphing process to suit different tasks and environments, and in designing systems that combine reversible actuation and self-healing ability. Here, we report halogen-bonded liquid crystal elastomers (LCEs) that can be arbitrarily shape-programmed and that self-heal under mild thermal or photothermal stimulation. We incorporate halogen-bond-donating diiodotetrafluorobenzene molecules as dynamic supramolecular crosslinks into the LCEs and show that these relatively weak crosslinks are pertinent for their mechanical programming and self-healing. Utilizing the halogen-bonded LCEs, we demonstrate proof-of-concept soft robotic motions such as crawling and rolling with programmed velocities. Our results showcase halogen bonding as a promising, yet unexplored tool for the preparation of smart supramolecular constructs for the development of advanced soft actuators.  相似文献   
979.
The migration of ions is known to be associated with various detrimental phenomena, including current density-voltage hysteresis, phase segregation, etc., which significantly limit the stability and performance of perovskite solar cells, impeding their progress toward commercial applications. To address these challenges, we propose incorporating a polymerizable organic small molecule monomer, N-carbamoyl-2-propan-2-ylpent-4-enamide (Apronal), into the perovskite film to form a crosslinked polymer (P-Apronal) through thermal crosslinking. The carbonyl and amino groups in Apronal effectively interact with shallow defects, such as uncoordinated Pb2+ and iodide vacancies, leading to the formation of high-quality films with enhanced crystallinity and reduced lattice strain. Furthermore, the introduction of P-Apronal improves energy level alignment, and facilitates charge carrier extraction and transport, resulting in a champion efficiency of 25.09 %. Importantly, P-Apronal can effectively suppress the migration of I ions and improve the long-term stability of the devices. The present strategy sets forth a path to attain long-term stability and enhanced efficiency in perovskite solar cells.  相似文献   
980.
Recent reports on the formation of hydrogen peroxide (H2O2) in water microdroplets produced via pneumatic spraying or capillary condensation have garnered significant attention. How covalent bonds in water could break under such mild conditions challenges our textbook understanding of physical chemistry and water. While there is no definitive answer, it has been speculated that ultrahigh electric fields at the air–water interface are responsible for this chemical transformation. Here, we report on our comprehensive experimental investigation of H2O2 formation in (i) water microdroplets sprayed over a range of liquid flow-rates, (shearing) air flow rates, and air composition, and (ii) water microdroplets condensed on hydrophobic substrates formed via hot water or humidifier under controlled air composition. Specifically, we assessed the contributions of the evaporative concentration and shock waves in sprays and the effects of trace O3(g) on the H2O2 formation. Glovebox experiments revealed that the H2O2 formation in water microdroplets was most sensitive to the air–borne ozone (O3) concentration. In the absence of O3(g), we could not detect H2O2(aq) in sprays or condensates (detection limit ≥250 nM). In contrast, microdroplets exposed to atmospherically relevant O3(g) concentration (10–100 ppb) formed 2–30 µM H2O2(aq), increasing with the gas–liquid surface area, mixing, and contact duration. Thus, the water surface area facilitates the O3(g) mass transfer, which is followed by the chemical transformation of O3(aq) into H2O2(aq). These findings should also help us understand the implications of this chemistry in natural and applied contexts.

A. Gallo Jr, H. Mishra et al., pinpoint the origins of the spontaneous H2O2 formation in water microdroplets formed via spraying or condensation, i.e., without the addition of electrical energy, catalyst, or co-solvent.  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