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   1681篇
  免费   112篇
  国内免费   145篇
化学   1311篇
晶体学   41篇
力学   94篇
综合类   9篇
数学   19篇
物理学   464篇
  2024年   4篇
  2023年   16篇
  2022年   43篇
  2021年   47篇
  2020年   57篇
  2019年   51篇
  2018年   45篇
  2017年   60篇
  2016年   54篇
  2015年   66篇
  2014年   98篇
  2013年   136篇
  2012年   77篇
  2011年   147篇
  2010年   67篇
  2009年   94篇
  2008年   78篇
  2007年   116篇
  2006年   85篇
  2005年   82篇
  2004年   67篇
  2003年   67篇
  2002年   71篇
  2001年   38篇
  2000年   32篇
  1999年   50篇
  1998年   26篇
  1997年   25篇
  1996年   27篇
  1995年   26篇
  1994年   24篇
  1993年   10篇
  1992年   19篇
  1991年   6篇
  1990年   5篇
  1989年   4篇
  1988年   3篇
  1987年   2篇
  1986年   3篇
  1985年   2篇
  1984年   1篇
  1983年   3篇
  1981年   2篇
  1980年   1篇
  1966年   1篇
排序方式: 共有1938条查询结果,搜索用时 31 毫秒
91.
在内构件(传热板和中心集气管)外热式固定床反应器中研究了油页岩热解产物生成特性,并与无内构件的相同常规固定床反应器内的油页岩热解行为对比,考察了两反应器中油页岩升温特性、热解产物分布、页岩油品质以及气体产物组成的变化规律.结果表明,内置传热板和中心集气管显著强化了反应器内的传热,相对于无内构件常规固定床反应器,料层升温速率提高了约2倍.对于依兰油页岩,其热解页岩油产率明显提高,最高达11.1 wt%(干燥基),明显高于无构件常规固定床反应器获得的页岩油产率.随着外加热炉温度的升高,内构件固定床反应器的页岩油产率逐渐增加,而无内构件常规固定床反应器的页岩油产率则明显降低.当外加热炉温度为1000℃时,前者页岩油产率是后者的2.3倍,并且内构件固定床反应器的热解水产率较低.两反应器中热解气产物组成相近,其H2与CH4之和占气体总量的70 vol%左右,热值为4406~5400 kcal/Nm3.  相似文献   
92.
Spherical, hollow MnS? C composite powders were prepared from a solution of manganese salt, thiourea, and sucrose by one‐pot spray pyrolysis. The MnS? C composite powders were generated by direct sulfidation of MnO with hydrogen sulfide gas generated in situ by decomposition of thiourea during spray pyrolysis. Sucrose, which is used as a carbon source material, plays a key role in the formation of the MnS? C composite powders by improving the reducing atmosphere around the powders. Dot‐mapping images of the composite powders demonstrated uniform distribution of the manganese, sulfur, and carbon components within the MnS? C composite powder. Fine crystals of MnS were uniformly mixed with carbon derived from polymerization and carbonization of sucrose. The carbon content of the MnS? C composite powders was 26 wt %. The discharge capacities of the MnS? C composite powders in the 2nd and 200th cycles were 863 and 967 mA h g?1, respectively, at a current density of 1000 mA g?1. The spherical and hollow morphology of the MnS? C composite powders was completely retained, even after 200 cycles. The enhanced cycling and rate performance of the MnS? C composite powders is ascribed to the structural stability of the composite powders.  相似文献   
93.
In this study, we report the first preparation of phase‐pure Co9S8 yolk–shell microspheres in a facile two‐step process and their improved electrochemical properties. Yolk–shell Co3O4 precursor microspheres are initially obtained by spray pyrolysis and are subsequently transformed into Co9S8 yolk–shell microspheres by simple sulfidation in the presence of thiourea as a sulfur source at 350 °C under a reducing atmosphere. For comparison, filled Co9S8 microspheres were also prepared using the same procedure but in the absence of sucrose during the spray pyrolysis. The prepared yolk–shell Co9S8 microspheres exhibited a Brunauer–Emmett–Teller (BET) specific surface area of 18 m2 g?1 with a mean pore size of 16 nm. The yolk–shell Co9S8 microspheres have initial discharge and charge capacities of 1008 and 767 mA h g?1 at a current density of 1000 mA g?1, respectively, while the filled Co9S8 microspheres have initial discharge and charge capacities of 838 and 638 mA h g?1, respectively. After 100 cycles, the discharge capacities of the yolk–shell and filled microspheres are 634 and 434 mA h g?1, respectively, and the corresponding capacity retentions after the first cycle are 82 % and 66 %.  相似文献   
94.
High‐temperature flame spray pyrolysis is employed for finding highly efficient nanomaterials for use in lithium‐ion batteries. CoOx‐FeOx nanopowders with various compositions are prepared by one‐pot high‐temperature flame spray pyrolysis. The Co and Fe components are uniformly distributed over the CoOx‐FeOx composite powders, irrespective of the Co/Fe mole ratio. The Co‐rich CoOx‐FeOx composite powders with Co/Fe mole ratios of 3:1 and 2:1 have mixed crystal structures with CoFe2O4 and Co3O4 phases. However, Co‐substituted magnetite composite powders prepared from spray solutions with Co and Fe components in mole ratios of 1:3, 1:2, and 1:1 have a single phase. Multicomponent CoOx‐FeOx powders with a Co/Fe mole ratio of 2:1 and a mixed crystal structure with Co3O4 and CoFe2O4 phases show high initial capacities and good cycling performance. The stable reversible discharge capacities of the composite powders with a Co/Fe mole ratio of 2:1 decrease from 1165 to 820 mA h g?1 as the current density is increased from 500 to 5000 mA g?1; however, the discharge capacity again increases to 1310 mA h g?1 as the current density is restored to 500 mA g?1.  相似文献   
95.
96.
An aqueous colloidal dispersion of Pt nanoparticles (NPs) stabilized by fullerenol C60(OH)12 (Pt:C60(OH)12) was successfully synthesized via liquid-phase chemical reduction. The subsequent pyrolysis of Pt:C60(OH)12 at different temperatures was conducted to afford Pt-doped carbon with different chemical compositions (Pt:C60n). X-ray absorption spectroscopy (XAS) and Infrared (IR) absorption spectroscopy and thermogravimetric measurements revealed that the thus-prepared nanocomposite consists of Pt NPs and high valent Pt-C60(OH)12 complex. One distinct feature of C60(OH)12 matrix as catalyst support is the suppression of size growth of Pt NPs during the pyrolysis up to 300 °C. Electrochemical experiments using cyclic voltammetry (CV) and linear sweep voltammetry (LSV) were performed to find that Pt:C60300 (pyrolyzed at 300 °C) exhibited higher activity than others, that was attributed to the π-extended feature of the as-obtained carbon.  相似文献   
97.
"用普通氧化锌晶须作为原材料, 采用高压釜腐蚀法和高温(600 ℃)裂解结合的方法合成纳米棒构成的氧化锌类椭球结构.XRD、SEM和TEM结果表明这种类椭球结构是单晶的,纳米棒取向一致,自组装生长而成."  相似文献   
98.
This paper reports on transient dynamics of electrospray driven by high step voltage and its dependence on voltage rise time. Three rise times (50 ns, 1.8 μs, and 400 μs) were used to compare influence on liquid dynamics. It was found that, when the applied voltage exceeds a certain level, minute differences in voltage rise time significantly affect jet formation time. A rise time of 50 ns accelerates the jet ejection by about 20% compared with other rise times. These results indicate that optimization of rise time may enable drastic improvement of controllability of drop-on-demand electrospray.  相似文献   
99.
Knowledge of the major effects governing desorption/ionization efficiency is required for the development and application of ambient mass spectrometry. Although all triacylglycerols (TAG) have the same favorable protonation and cationization sites, their desorption/ionization efficiencies can vary dramatically during easy ambient sonic‐spray ionization because of structural differences in the carbon chain. To quantify this somewhat surprising and drastic effect, we have performed a systematic investigation of desorption/ionization efficiencies as a function of unsaturation and length for TAG as well as for diacylglycerols, monoacylglycerols and several phospholipids (PL). Affinities for Na+ as a function of unsaturation level have also been assayed via comprehensive metadynamics calculations to understand the influence of this phenomenon on the ionization efficiency. The results suggest that dipole–dipole interactions within a carbon chain tuned by unsaturation sites govern ionization efficiency of TAG and PL. Copyright © 2014 John Wiley & Sons, Ltd.  相似文献   
100.
In this study, alleviation of ion suppression effect in sonic spray ionization mass spectrometry (SSI‐MS) was investigated. Ion suppression effect was firstly compared between electrospray ionization (ESI) and conventional SSI, and more severe ion suppression effect was observed with SSI. Ion suppression effect of SSI was also found difficult to be alleviated by simply optimizing major parameters. Alternatively, we found that with the assistance of an alternating current (AC) voltage with low amplitude, the ion suppression effect was greatly alleviated (comparable with conventional ESI). That AC voltage was applied outside the SSI spray tip, and no direct contact between the electrode and spray solution was necessary. Besides the alleviation of the ion suppression effect, this newly‐developed method, termed as induced electrosonic spray ionization (IESSI), appeared to preserve similar charge state distribution with SSI for protonated cytochrome c, hemoglobin, and bradykinin. IESSI could also obtain significantly improved ion intensities (~1000‐fold over conventional SSI). In addition, tolerance of concentrated salts for IESSI‐MS was investigated through the analysis of cytochrome c in the presence of concentrated sodium chloride (NaCl) or ammonium acetate (NH4OAc). Copyright © 2014 John Wiley & Sons, Ltd.  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