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Form selection of concomitant polymorphs: A case study informed by crystallization kinetics modeling
Weiwei Tang Yufeng Quan Junbo Gong Jingkang Wang Qiuxiang Yin Tonglei Li 《American Institute of Chemical Engineers》2021,67(4):e17129
Molecular mechanisms and process kinetics of crystallizing concomitant polymorphs remain poorly understood. Solvent-mediated phase transformation and concomitant crystallization are difficult to be distinguished in practice, as multiple forms can be detected at the same time. Herein, we developed a population balance model to simulate a concomitant crystallization process of two polymorphs of tolfenamic acid. Our kinetic modeling aims to understand concomitant crystallization and help guide form selection of such a molecular system. Crystallization kinetics of ethanolic solutions were uncovered from induction time measurements, as well as seeded and unseeded crystallization experiments. Experimental and simulation results demonstrate that the stable form I crystallizes concomitantly with the metastable form II. The faster growing form II results in an intermediate decline in the composition of form I in crystallized samples, a characteristic feature of the concomitantly crystallized system. A four-quadrant scheme of attainable polymorph outcome was simulated under various crystallization conditions. 相似文献
3.
Lingping Kong Jue Gong Qingyang Hu Francesco Capitani Anna Celeste Takanori Hattori Asami Sano-Furukawa Nana Li Wenge Yang Gang Liu Ho-kwang Mao 《Advanced functional materials》2021,31(9):2009131
The soft nature of organic–inorganic halide perovskites renders their lattice particularly tunable to external stimuli such as pressure, undoubtedly offering an effective way to modify their structure for extraordinary optoelectronic properties. Here, using the methylammonium lead iodide as a representative exploratory platform, it is observed that the pressure-driven lattice disorder can be significantly suppressed via hydrogen isotope effect, which is crucial for better optical and mechanical properties previously unattainable. By a comprehensive in situ neutron/synchrotron-based analysis and optical characterizations, a remarkable photoluminescence (PL) enhancement by threefold is convinced in deuterated CD3ND3PbI3, which also shows much greater structural robustness with retainable PL after high peak-pressure compression–decompression cycle. With the first-principles calculations, an atomic level understanding of the strong correlation among the organic sublattice and lead iodide octahedral framework and structural photonics is proposed, where the less dynamic CD3ND3+ cations are vital to maintain the long-range crystalline order through steric and Coulombic interactions. These results also show that CD3ND3PbI3-based solar cell has comparable photovoltaic performance as CH3NH3PbI3-based device but exhibits considerably slower degradation behavior, thus representing a paradigm by suggesting isotope-functionalized perovskite materials for better materials-by-design and more stable photovoltaic application. 相似文献
4.
The Fe/C/SiCN composite ceramics were synthesized by polymer-derived method to obtain the integration of structure and functions. The electromagnetic waves (EMW) absorption properties at X and Ku bands were investigated. The addition of nano-sized Fe particles improved the magnetic loss and impedance matching, and the carbon nanotubes generated by the iron in-situ catalysis increased the internal relaxation polarization and interfacial polarization, which together improved the EMW absorption properties significantly. In particular, the Fe/C/SiCN-9 showed the optimum reflection loss (RL) of ?31.06 dB at 10.03 GHz with an effective absorption bandwidth (EAB, RL < ?10 dB) of 3.03 GHz at 2.51 mm, indicating the excellent EMW absorption properties of Fe/C/SiCN composite ceramics. 相似文献
5.
Pu Mao Jiping Wang Peng Xiao Lixue Zhang Fang Kang Hao Gong 《Ceramics International》2021,47(1):111-120
In this work, we developed a novel system of isovalent Zr4+ and donor Nb5+ co-doped CaCu3Ti4O12 (CCTO) ceramics to enhance dielectric response. The influences of Zr4+ and Nb5+ co-substituting on the colossal dielectric response and relaxation behavior of the CCTO ceramics fabricated by a conventional solid-phase synthesis method were investigated methodically. Co-doping of Zr4+ and Nb5+ ions leads to a significant reduction in grain size for the CCTO ceramics sintered at 1060 °C for 10 h. XRD and Raman results of the CaCu3Ti3.8-xZrxNb0.2O12 (CCTZNO) ceramics show a cubic perovskite structure with space group Im-3. The first principle calculation result exhibits a better thermodynamic stability of the CCTO structure co-doped with Zr4+ and Nb5+ ions than that of single-doped with Zr4+ or Nb5+ ion. Interestingly, the CCTZNO ceramics exhibit greatly improved dielectric constant (~105) at a frequency range of 102–105 Hz and at a temperature range of 20–210 °C, indicating a giant dielectric response within broader frequency and temperature ranges. The dielectric properties of CCTZNO ceramics were analyzed from the viewpoints of defect-dipole effect and internal barrier layer capacitance (IBLC) model. Accordingly, the immensely enhanced dielectric response is primarily ascribed to the complex defect dipoles associated with oxygen vacancies by co-doping Zr4+ and Nb5+ ions into CCTO structure. In addition, the obvious dielectric relaxation behavior has been found in CCTZNO ceramics, and the relaxation process in middle frequency regions is attributed to the grain boundary response confirmed by complex impedance spectroscopy and electric modulus. 相似文献
6.
Yan Liu Qian Wu Zhenzhen Xia Yang Wu Yan Li Zhiyong Gong 《Journal of the science of food and agriculture》2020,100(12):4418-4424
7.
镜铁山矿Ⅰ#矿体向下延伸时倾角由急倾斜变为倾斜,若继续按照急倾斜矿体的回采方式布置采切工程,将会在矿体上盘或者下盘处残留三角形边角矿,进而导致矿石损失率增大。为有效解决因矿体倾角缓化出现的三角区域矿体难以回收的问题,首先提出了脉内布置分段沿脉巷和沿矿岩边界布置分段沿脉巷两类回采方案,其中脉内布置分段沿脉巷回采方案设计了15°、30°、45° 3种不同中深孔边孔角布置方案;然后分别从中深孔施孔精度要求、中深孔施工适应性、对矿体条件适应性、生产效率等4个方面定性分析了不同回采方案的优劣性;最后整合生产效率、施工适应性、通风效果、井巷工程量、工期和成本等12个指标组成优选评价体系,采用层次分析法(Analytic Hierarchy Process,AHP)构建了倾斜矿体上盘边角矿回采方案层次分析优选模型。计算得到3种脉内布置分段沿脉巷与沿矿岩边界布置回采方案的最终评价值分别为0.213、0.201、0.198和0.388,结果表明:沿矿岩边界布置分段沿脉巷为最优回采方案。实践表明:优选出的方案在实践中取得了理想效果,经济效益显著,可满足该矿倾斜矿体上盘边角矿回采需求。研究结果可为类似开采条件矿山的边角矿回采提供有益参考。 相似文献
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9.
This study examined airborne emissions from cigarette butts for styrene, 2-methyl-2-cyclopenten-1-one, naphthalene, triacetin, and nicotine. Ten experiments were conducted by placing butts in a stainless steel chamber and measuring the chemical concentrations in chamber air. Emission rates were determined from the concentrations. Triacetin and nicotine concentrations were roughly 50% of initial concentrations after 100 hours, while concentrations of other chemicals decayed to less than 10% of initial concentrations within 24 hours. Initial emission rates per cigarette butt ranged from 200 to 3500 ng h−1. Triacetin and nicotine emission rates at 25°C were 1.6 to 2.2 times higher than the rates at 20°C, while the emission rates of other chemicals at 25°C were 1.1 to 1.3 times higher than the rates at 20°C only during the first sampling period. The chemical concentrations and emission rates at 30°C were comparable or lower than the values at 25°C, possibly due to different batches of cigarettes used. The 24-hours emitted mass of nicotine from a cigarette butt at 25°C could be up to 14% of the literature reported nicotine masses emitted from a burning cigarette. 相似文献
10.
Experimental and simulation studies on the migration characteristics of heavy metals during the incineration of OS were conducted with a tube furnace reactor and thermodynamic equilibrium calculation software FactSage, respectively. The results showed that when the incineration temperature increased from 800°C to 1100°C, the release rates of heavy metals such as Cr, Pb, Cu, Zn and Ni increased gradually and reached the maximum at 1000°C. When the excess air ratio increased from 1.0 to 1.4, the release rates of heavy metals such as Cr, Pb, Cu, Zn and Ni first decreased and then became steady. The content of gaseous hydroxide of Cr and gaseous chlorides of Pb and Cu increased while the chemical forms of Zn and Ni did not change obviously with the increase of combustion temperature or excess air ratio. 相似文献