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1.
Minh Nguyen Vo Jonathan P. Ruffley J. Karl Johnson 《American Institute of Chemical Engineers》2021,67(3):e17156
Metal organic frameworks (MOFs) containing zirconium secondary building units (SBUs) in UiO-67 and related MOFs, are highly active for neutralizing both the chemical warfare agents and simulants, such as dimethyl methylphosphonate (DMMP). However, two recent publications gave conflicting reports of DMMP reaction with UiO-67 under ultra high vacuum (UHV) conditions, with one reporting chemisorption and reaction (Wang et al., J Phys Chem C, 2017, 121, 11261–11272) and the other reporting only physisorption and reversible desorption (Ruffley et al., J Phys Chem C, 2019, 123, 19748–19758) from very similar temperature programmed desorption experiments. We show that the discrepancy between these experiments may be explained by different levels of missing linker defects in the UiO-67 samples. We present density functional theory calculations showing that SBU sites having two-adjacent missing linkers exhibit reaction barriers that are about 30 kJ/mol lower than SBU sites having a single missing linker. We also show that topology of the undercoordinated sites plays an important role in the reaction barrier under UHV conditions. 相似文献
2.
Ib Holzmeister Jan Weichhold Jürgen Groll Hala Zreiqat Uwe Gbureck 《Journal of the American Ceramic Society》2021,104(7):3554-3561
In this study, the hydraulic reactivity and cement formation of baghdadite (Ca3ZrSi2O9) was investigated. The material was synthesized by sintering a mixture of CaCO3, SiO2, and ZrO2 and then mechanically activated using a planetary mill. This leads to a decrease in particle and crystallite size and a partial amorphization of baghdadite as shown by X-ray powder diffraction (XRD) and laser diffraction measurements. Baghdadite cements were formed by the addition of water at a powder to liquid ratio of 2.0 g/ml. Maximum compressive strengths were found to be ~2 MPa after 3-day setting for a 24-h ground material. Inductively coupled plasma mass spectrometry (ICP-MS) measurements showed an incongruent dissolution profile of set cements with a preferred dissolution of calcium and only marginal release of zirconium ions. Cement formation occurs under alkaline conditions, whereas the unground raw powder leads to a pH of 11.9 during setting, while prolonged grinding increased pH values to approximately 12.3. 相似文献
3.
Characteristics of reaction and product microstructure during light calcination of magnesite in transport bed 下载免费PDF全文
A gas-heating laboratory transport bed was adopted to simulate the industrial transportbed reactor for flash calcination of magnesite, and a method based on TG analysis of a reacted sample was further developed to calculate the decomposition rate or conversion of its containing MgCO3. The study investigated how the conversion and product reactivity as well as microstructure vary with reaction conditions including temperature, particle size and times of re-calcination for powder magnesite. Magnesite powder (<150 μm) calcination is a quick reaction that reaches 98% decomposition of its containing MgCO3 in 1—2 s,corroborating the feasibility of magnesite flash-calcination in transport bed reactors. The coloration time given by the citric acid chromogenic method was 17—55 s and 294 s for the obtained products from transport and fixed beds, respectively. This proves the obviously higher activity and thus improved microstructure of the product from transport bed. During the calcination process, the MgO grain size of the product gradually increases, and the surface structure changes from loose and porous to dense and smooth. This structural change can be completed within a few seconds. 相似文献
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The fashionable Parr–Pearson (PP) atoms-in-molecule/bonding (AIM/AIB) approach for determining the exchanged charge necessary for acquiring an equalized electronegativity within a chemical bond is refined and generalized here by introducing the concepts of chemical power within the chemical orthogonal space (COS) in terms of electronegativity and chemical hardness. Electronegativity and chemical hardness are conceptually orthogonal, since there are opposite tendencies in bonding, i.e., reactivity vs. stability or the HOMO-LUMO middy level vs. the HOMO-LUMO interval (gap). Thus, atoms-in-molecule/bond electronegativity and chemical hardness are provided for in orthogonal space (COS), along with a generalized analytical expression of the exchanged electrons in bonding. Moreover, the present formalism surpasses the earlier Parr–Pearson limitation to the context of hetero-bonding molecules so as to also include the important case of covalent homo-bonding. The connections of the present COS analysis with PP formalism is analytically revealed, while a numerical illustration regarding the patterning and fragmentation of chemical benchmarking bondings is also presented and fundamental open questions are critically discussed. 相似文献
6.
木质素是自然界储量丰富的可再生天然酚类高分子,可替代传统化石资源应用于聚合物材料合成。木质素分子结构中的大分子刚性骨架可赋予材料独特的力学性能和热稳定性。但木质素化学组成和分子结构复杂、反应活性低,限制了在聚合物材料领域的应用。化学降解是一种高效、高选择性且应用广泛的降解方法,经化学降解处理得到的木质素低聚物具有活性官能团多、反应活性高、溶解性好等优点,有利于拓展木质素在聚合物材料领域的高附加值应用。重点综述了近年来国内外有关木质素化学降解及其降解产物应用于聚合物材料的研究进展。 相似文献
7.
碳酸甲乙酯(EMC)是一种环境友好型的不对称碳酸酯,因其独特的结构性质被广泛用作溶剂或有机合成中间体,特别是随着锂离子电池的迅猛发展,其作为电池电解液主要成分市场需求量急增。文中简单介绍了光气法、氧化羰化法和酯交换法合成碳酸甲乙酯的研究进展。重点针对最具发展前景的酯交换法合成EMC工艺路线中所用催化剂进行了综述;讨论和分析了该路线所用催化剂的类型、结构、性质及性能,并对当前研究中存在的问题进行了归纳和分析总结。最后本文分析并展望了酯交换法合成EMC催化剂的研究方向及新型合成工艺发展趋势,提出研发经济、高效、稳定且制备工艺简单的非均相催化剂,并与反应精馏技术耦合是今后的主要发展趋势,期望为EMC的高效合成提供参考和借鉴。 相似文献
8.
Combining the Su–Schrieffer–Heeger and Pariser–Parr–Pople model (SSH+PPP), we have studied the influence of electron–electron interactions on the motion and dissociation of a polaron in the presence of an electric field, with emphasis on the long-range Coulomb interactions. The multiconfigurational time-dependent Hartree–Fock (MCTDHF) formalism was used to compute the electron–electron interactions. How the saturated velocity and the critical dissociation electric field of the polaron are related to the on-site Coulomb repulsion and long-range Coulomb interactions has been investigated. It was found that the on-site Coulomb interaction does not favor the motion of a polaron. There is a critical strength of the long-range Coulomb interaction for which the polaron takes on the most localized configuration. Comparing with the results obtained using the extended Hubbard model, we found that competition between the long-range Coulomb interactions and the on-site Coulomb interaction leads to a non-monotonic dependence of both the saturated velocity and the critical dissociation electric field on the long-range Coulomb interactions. 相似文献
9.
Nuclear power plant Safety analysis using coupled 3D neutron kinetics/thermal-hydraulic codes technique is increasingly used nowadays. Actually, the use of this technique allows getting less conservatism and more realistic simulations of the physical phenomena. The challenge today is oriented toward the application of this technique to the operating conditions of nuclear research reactors. In the current study, a three-Dimensional Neutron Kinetics and best estimate Thermal-Hydraulic model based upon the coupled PARCS/RELAP5 codes has been developed and applied for a heavy water research reactor. The objective is to perform safety analysis related to design accidents of this reactor types. In the current study two positive reactivity insertion transients are considered, SCRAM protected and self-limiting power excursion cases. The results of the steady state calculations were compared with results obtained from conventional diffusion codes, while transient calculations were assessed using the point kinetic model of the RELAP5 code. Through this study, the applicability and the suitability of using the coupled code technique with respect to the classical models are emphasized and discussed. 相似文献
10.
Marcus Heinze Sandra Starke Marcel Händler Hartmut Komber Marco Drache Norbert Moszner Brigitte Voit Doris Pospiech 《应用聚合物科学杂志》2019,136(48):48256
We demonstrate in this study that the combination of modern inline monitoring methods [here: inline nuclear magnetic resonance (NMR)] with simulations gains more exact and profound kinetic results than previously used methods like linearization without that combination. The 1H-NMR spectroscopic data (more than 100 data points) are used to construct the copolymerization diagram. The reactivity ratios are obtained applying the van Herks nonlinear least square method. The examination of the radical copolymerization of 2-hydroxyethyl methacrylate (HEMA) with (2-{[2-(ethoxycarbonyl)prop-2-en-1-yl]oxy}ethyl) phosphonic acid (ECPPA) as important adhesive monomer used in dentistry yields reactivity ratios of rHEMA = 1.83; rECPPA = 0.42. The copolymerization diagram reflects nonideal, non-azeotropic copolymerization. The sequence distribution of the obtained by Monte Carlo simulation indicates the generation of statistical copolymers. As an important finding, it is demonstrated that the repeating units responsible for etching and adhesion are arranged over the whole polymer chain, which is necessary to achieve proper functionality. © 2019 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2019 , 136, 48256. 相似文献