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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.
Bryan D. Paulsen Ruiheng Wu Christopher J. Takacs Hans-Georg Steinrück Joseph Strzalka Qingteng Zhang Michael F. Toney Jonathan Rivnay 《Advanced materials (Deerfield Beach, Fla.)》2020,32(40):2003404
The structure and packing of organic mixed ionic–electronic conductors have an especially significant effect on transport properties. In operating devices, this structure is not fixed but is responsive to changes in electrochemical potential, ion intercalation, and solvent swelling. Toward this end, the steady-state and transient structure of the model organic mixed conductor, poly(3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS), is characterized using multimodal time-resolved operando techniques. Steady-state operando X-ray scattering reveals a doping-induced lamellar expansion of 1.6 Å followed by 0.4 Å relaxation at high doping levels. Time-resolved operando X-ray scattering reveals asymmetric rates of lamellar structural change during doping and dedoping that do not directly depend on potential or charging transients. Time-resolved spectroscopy establishes a link between structural transients and the complex kinetics of electronic charge carrier subpopulations, in particular the polaron–bipolaron equilibrium. These findings provide insight into the factors limiting the response time of organic mixed-conductor-based devices, and present the first real-time observation of the structural changes during doping and dedoping of a conjugated polymer system via X-ray scattering. 相似文献
4.
The recent trend of aging population, not to mention the unprecedented pandemic, draws great attention from the general public about health concerns. Since healthcare information technology is different from non-healthcare information technology, additional contexts should be properly incorporated into technology acceptance research to accurately identify influential factors affecting the acceptance of wearable healthcare technology. Thus, we selectively reconfigured factors from health, privacy, and socio-demographic contexts to formulate a health-aware acceptance model. Then, it was empirically analyzed using structural equation modeling. Based on the results, whereas privacy concerns were directly associated with intention to use wearable healthcare technology, health concerns were not. Moreover, age had a moderating effect on social influence and facilitating conditions. These findings suggest valuable insights that the adoption rate of healthcare technology is increased by 1) keeping personal information securely, 2) facilitating social interaction among users, and 3) offering intuitive user experience for elderly people. 相似文献
5.
目的 了解武汉市一般人群血清中全氟及多氟烷基化合物(PFASs)浓度,探索血清中PFASs浓度水平的影响因素。方法 以在武汉市某医院进行一般体检的人群为研究对象(n=67),通过超高效液相色谱-三重四级杆质谱(UPLC-TQ/MS)联用仪测定外周血清中12种PFASs浓度,采用多元线性回归分析方法分析一般人口学特征和血清中PFASs浓度的关联性。结果 武汉市一般人群血清中12种PFASs的平均浓度水平为11.60 ng/mL。全氟辛烷磺酸及其盐类(PFOS)和全氟辛酸及其盐类(PFOA)的贡献率较大,分别为45.03%和31.86%。男性人群血清中PFOS、PFOA、全氟己基磺酸(PFHxS)、全氟壬酸(PFNA)等主要化合物的浓度高于女性,其β值(95%可信区间)分别为0.708(0.313,1.104)、0.518(0.069,0.967)、0.724(0.388,1.059)和0.684(0.399,0.968)。同时,发现血清中PFOS、PFHxS、PFNA浓度和年龄呈正相关,其β值(95%可信区间)分别为0.062(0.042,0.081)、0.035(0.019,0.052)和0.030(0.016,0.045)。结论 性别和年龄对血清中PFASs浓度有影响,在进行人体PFASs暴露评估中应考虑这些因素。 相似文献
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7.
Persisters are drug-tolerant bacteria that account for the majority of bacterial infections. They are not mutants, rather, they are slow-growing cells in an otherwise normally growing population. It is known that the frequency of persisters in a population is correlated with the number of toxin–antitoxin systems in the organism. Our previous work provided a mechanistic link between the two by showing how multiple toxin–antitoxin systems, which are present in nearly all bacteria, can cooperate to induce bistable toxin concentrations that result in a heterogeneous population of slow- and fast-growing cells. As such, the slow-growing persisters are a bet-hedging subpopulation maintained under normal conditions. For technical reasons, the model assumed that the kinetic parameters of the various toxin–antitoxin systems in the cell are identical, but experimental data indicate that they differ, sometimes dramatically. Thus, a critical question remains: whether toxin–antitoxin systems from the diverse families, often found together in a cell, with significantly different kinetics, can cooperate in a similar manner. Here, we characterize the interaction of toxin–antitoxin systems from many families that are unrelated and kinetically diverse, and identify the essential determinant for their cooperation. The generic architecture of toxin–antitoxin systems provides the potential for bistability, and our results show that even when they do not exhibit bistability alone, unrelated systems can be coupled by the growth rate to create a strongly bistable, hysteretic switch between normal (fast-growing) and persistent (slow-growing) states. Different combinations of kinetic parameters can produce similar toxic switching thresholds, and the proximity of the thresholds is the primary determinant of bistability. Stochastic fluctuations can spontaneously switch all of the toxin–antitoxin systems in a cell at once. The spontaneous switch creates a heterogeneous population of growing and non-growing cells, typical of persisters, that exist under normal conditions, rather than only as an induced response. The frequency of persisters in the population can be tuned for a particular environmental niche by mixing and matching unrelated systems via mutation, horizontal gene transfer and selection. 相似文献
8.
Florian Meierhofer Lutz Mädler Udo Fritsching 《American Institute of Chemical Engineers》2020,66(2):e16885
In flame spray pyrolysis (FSP), the evolution of metal oxide nanoparticles relies on quite a number of droplet (liquid) and vapor phase related physical mechanism as for instance precursor evaporation, oxidation, nucleation via gas-to-particle conversion mechanism, and subsequent particle (solid) growth mechanisms based on coagulation, sintering/coalescence, and agglomeration. The liquid precursor and dispersion oxygen feed rates are relevant control parameters of the FSP process for tailoring the nanoparticle size (diameter) and structure as well as the atomizer nozzle configuration. Sophisticated nonintrusive, laser-based in situ and ex situ diagnostics with multiscale spatial resolution (micrometer to meter range) are applied for analyzing droplet formation and size, gas velocity, temperature, species concentration, as well as primary and agglomerate diameters along the flow direction. Computational fluid dynamics (CFD) are coupled with population balance modeling (PBM) to elucidate the nanoparticle dynamics within the reactive spray. It is found that the CFD-PBM approach allows estimations of primary and agglomerate nanoparticle diameters within 80 and 75% accuracy compared to experimental data, suggesting that the methods presented could pave the way for designing next-generations of flame reactors. 相似文献
9.
Caio Felippe Curitiba Marcellos Camila M. Senna Figueiredo Frederico W. Tavares Maurício Bezerra de Souza Jr. Paulo Laranjeira da Cunha Lage João Francisco Cajaiba da Silva Argimiro R. Secchi Amaro G. Barreto Jr. 《加拿大化工杂志》2020,98(11):2435-2450
An experimental methodology for inferring brine dissolution rate in monoethylene glycol (MEG) solutions at different temperatures using a webcam combined with a mathematical model is presented. The measurement system is designed to track the RGB (red, green, and blue) colour variations during the dissolution process. A dynamic model augmented with the population balance equation is applied to describe the dissolution process. Moreover, the dissolution rate is consistently related to the temperature and MEG concentration through the driving force based on the Gibbs energy and chemical affinity. The applied low-cost measurement apparatus proved to be a useful resource for tracking the dissolution dynamics in a wide range of undersaturation. 相似文献
10.
针对滚动轴承振动信号具有非线性、非平稳性和非高斯性,并且故障特征往往淹没于系统噪声之中而难于识别的问题,
提出了以多种群差分进化(multiple population differential evolution, MPDE) 算法来改进集合经验模式分解( ensemble empirical
mode decomposition, EEMD) 的 MPDE-EEMD 消噪方法,并与自适应共振解调技术( adaptive resonance demodulation technique,
ARDT)相结合实现故障特征提取。 首先,为了解决 EEMD 中加入参数依靠人工选择且难以准确获取的问题,建立极值点分布
特性评价函数,利用 MPDE 来寻优获取最佳白噪声幅值,实现 EEMD 自适应分解。 然后,采用峭度与相关性相结合的准则对分
解后的 IMF 分量进行自动筛选,将满足条件的有效信号进行重构,实现对原始振动信号的降噪处理。 最后,采用 ARDT 自动确
定对消噪信号进行带通滤波的带宽和中心频率,再通过包络解调提取出滤波信号的特征频率。 将轴承仿真故障信号与实际故
障信号用于算法的验证,结果表明 MPDE-EEMD+ARDT 能有效提取出轴承故障特征。 相似文献