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Designing low-cost, highly efficient, and durable electrocatalysts for carbon dioxide reduction reaction (eCO2RR) to value-added chemicals is an appealing approach to balance the global carbon emission. Heterogeneous molecular catalysts is emerging as an important area for CO2 utilization. Herein, a series of atomically isolated transition metal-N4 sites anchored on porphyrin framework (TM/PRF) molecular catalysts are employed as electrocatalysts for eCO2RR because of their well-defined structure, the versatility and relatively low cost, and remarkable activity, which allow the establishment of precise structural model for a better understanding of the CO2 reduction mechanism. Based on density functional theory calculations and the computational hydrogen electrode model on 27 candidates, we propose a number of TM/PRF (TMs = Ni, Co, Mn, Cu, Ag, Au, Zn, Pd, Ti, V, Cr, Ta, W), which show promise of highly active and selective catalysts for carbon monoxide, formic acid, methane and methanol production, while simultaneously suppress competing hydrogen evolution reaction. Studies have shown that the TM center plays a crucial role in determining the catalytic performance of the material. And the TM/PRF molecule tends to stabilize different radical intermediates at the TM site. Thus, when reacted with a greater number of electrons, highly reduced products are formed. Among the different TM/PRF materials, Ta/PRF and W/PRF have been shown to produce CH3OH selectively at low overpotentials (0.39 and 0.58 V), whereas Ti/PRF has been found as highly selective toward CH4 production with low overpotential of 0.58 V, outperforming most known electrodes. The calulation of activation energy and the d-band center reveal that Cr/PRF shows higher catalystic activity in comparison with other TM/PRF. The advantages of the outstanding selectivity of products, the reduced overpotentials and the higher activity of catalyst allow these new systems TM/PRF (TMs = Ta, W, Ti, Cr) to be promising catalysts, which will motivate more fundamental mechanism studies and technological applications for eCO2RR. 相似文献
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Multi-factor authentication (MFA) was proposed by Pointcheval et al. [Pointcheval
and Zimmer (2008)] to improve the security of single-factor (and two-factor) authentication.
As the backbone of multi-factor authentication, biometric data are widely observed. Especially,
how to keep the privacy of biometric at the password database without impairing efficiency is
still an open question. Using the vulnerability of encryption (or hash) algorithms, the attacker
can still launch offline brute-force attacks on encrypted (or hashed) biometric data. To address
the potential risk of biometric disclosure at the password database, in this paper, we propose a
novel efficient and secure MFA key exchange (later denoted as MFAKE) protocol leveraging
the Pythia PRF service and password-to-random (or PTR) protocol. Armed with the PTR
protocol, a master password pwd can be translated by the user into independent pseudorandom
passwords (or rwd) for each user account with the help of device (e.g., smart phone).
Meanwhile, using the Pythia PRF service, the password database can avoid leakage of the
local user’s password and biometric data. This is the first paper to achieve the password and
biometric harden service simultaneously using the PTR protocol and Pythia PRF. 相似文献
25.
结合已有的超宽带(UWB)信号对全球定位系统(GPS)接收机的干扰实验,分析了不同脉冲重复频率(PRF)的超宽带脉冲信号对全球定位系统的潜在干扰.这些干扰主要是对中心频率为1176.45±12MHz的GPS接收机. 相似文献
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基于用加速量热仪(ARC)对参比燃料与空气的混合物在低温条件下的氧化特性的实验结果,对ARC实验结果进行了热力学和化学动力学分析.根据能量平衡方程,推导出在较小的样品质量下,考虑到密闭容器中各种基本反应物质的比热容随温度变化时,热惰性因子的准确表达式,算出参比燃料在反应过程中的实际自放热率,并根据化学动力学分析求出正庚烷和异辛烷低温氧化动力学参数.对正庚烷和异辛烷的自放热率分析发现,它们都出现双峰现象,并分别在589.4K和585.7K时有最大放热率,随后在598.5K和594.8K结束自放热. 相似文献
28.
ABSTRACT: Real-time temperature maps of ohmically heated liquid-particulate mixtures were acquired using the Proton Resonance Frequency (PRF) shift method incorporated into a fast Magnetic Resonance Imaging (MRI). Noise in the MRI images induced by the electrical heating power was eliminated by a post-processing algorithm of the PRF shift method and correction phase images. The time-dependent interface heat transfer coefficients ( hfp ) were determined during the holding period using the MRI temperature maps and numerical solutions to the Fourier's 2nd law. The calculated values of hfp range from 30 to 105 W/m2 K, consistent with literature values for natural convection. These results provide crucial data for understanding the ohmic heating process. 相似文献
29.
传统的伪相关反馈(Pseudo Relevance Feedback, PRF)方法通常是以文档作为扩展源单元提取扩展词,提取粒度过大造成扩展源质量下降,使得检索结果鲁棒性差。该文研究利用主题分析技术,尝试将文本语义内容作为扩展源单元,缓解扩展源质量不高的问题。提出并实现了对文本集中各文档内容的伪文档描述,通过对其进行隐式多样化处理,实现了从更细微的文本内容角度出发提取扩展词。通过在真实NTCIR8中文语料的检索结果表明,该方法可以有效地提升伪相关反馈的检索性能。 相似文献
30.