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71.
铜-配体(L)-三肽组成的三元复合物[Cu(L)M]2+,其中,L表示4′-氯-2,2′:6′,2″-三联吡啶(缩写为4Cl-tpy);M表示酪氨酰-甘氨酰-色氨酸(YGW)及其修饰型三肽(CH3CO-YGW-OCH3,缩写 Ac-YGW-OMe)。使用该复合物,通过碰撞诱导解离 (collision-induced dissociation, CID)产生两种自由基离子 ([YGW]·+和[Ac-YGW-OMe]·+)。采用串联质谱结合密度泛函理论 (density functional theory, DFT)得到气相稳定结构,并研究其气相解离行为。研究结果表明,[YGW]·+和[Ac-YGW-OMe]·+的气相解离行为截然不同,[YGW]·+主要产生[M-CO2-116]+和[M-CO2]·+碎片离子;而[Ac-YGW-OMe]·+在气相中主要产生[M-CH3OH]·+碎片离子。推测这两种离子的气相裂解机理分别为:[YGW]·+羧基上的质子重排到多肽骨架中羰基氧上,经历 Cα-C键的断裂产生[M-CO2]·+、断裂色氨酸侧链 Cβ-Cγ键产生[M-CO2-116]+离子;[Ac-YGW-OMe]·+则先经历质子重排到酯基氧上,然后经过C-O酯键的断裂形成[M-CH3OH]·+离子。参与重排的质子可能有3个来源:Ac-YGW-OMe中甘氨酸的Cα-H、色氨酸的Cα-H 或Cβ-H,该机理有待进一步验证。本研究将为其他类型多肽及衍生物的结构及气相反应机理研究提供参考。 相似文献
72.
针对工程形状设计领域中带有多个约束条件的非线性设计优化问题,提出了一种自适应的基于高斯分布的量子行为粒子群优化(AG-QPSO)算法。通过自适应地调整高斯分布,AG-QPSO算法能够在搜索的初始阶段有很强的全局搜索能力,随着搜索过程的进行,算法的局部搜索能力逐渐增强,从而满足了算法在搜索过程不同阶段的需要。为了验证算法的有效性,在压力容器和张弦设计问题这两个工程约束优化问题上进行50轮独立实验。实验结果表明,在满足所有约束条件的情况下,AG-QPSO算法在压力容器设计问题上取得了5890.9315的平均解和5885.3328的最优解,在张弦设计问题上取得了0.01096的平均解和0.01096的最优解,远优于标准粒子群优化(PSO)算法、具有量子行为的粒子群优化(QPSO)算法和高斯量子行为粒子群(G-QPSO)算法等现有的算法的结果,同时AG-QPSO算法取得的结果的方差较小,说明该算法具有很好的鲁棒性。 相似文献
73.
Bo Wu Huiying Du Ping Hu Zhanyu Gao Ruikai Liu Chonghua Pei 《Journal of Energetic Materials》2021,39(1):10-22
ABSTRACT In recent years, the exploration of a practical strategy for novel energetic molecules with high energy and low sensitivity is very desirable but highly challenging. Novel ionic energetic molecules have attracted much attention in this area due to their prominent advantages including low sensitivities, high thermal stability, and excellent energy performances. Herein, five different ionic energetic molecules based on new monovalent and divalent 4-oxyl-3,5-dinitropyrazolate moieties with enhanced oxygen balance have been synthesized, characterized and evaluated as potential high-energy materials. Thermal stability, sensitivities and energy output test were measured and studied in detail. The heats of formation and energetic parameters were calculated by using Gaussian 09 suite of programs and EXPLO 5 code. The results suggest that all as-prepared new molecules exhibit good thermal stability with high decomposition temperature (3, 231°C; 5, 160°C; 6, 185°C; 7, 180°C; 8, 213°C), and relative low sensitivity (IS > 20 J, FS = 324 N). Inheriting the significant oxygen content of monovalent and divalent 4-oxyl-3,5-dinitropyrazolate moieties, they also possess good energy properties (v D = 8238 ~ 9208 m s?1, P = 26.8 ~ 36.7 GPa, V o = 481.8 ~ 959.4 L kg?1), which make them competitive high-energy materials. 相似文献
74.
Khalid Quertite Hanna Enriquez Nicolas Trcera Yongfeng Tong Azzedine Bendounan Andrew J. Mayne Gérald Dujardin Pierre Lagarde Abdallah El kenz Abdelilah Benyoussef Yannick J. Dappe Abdelkader Kara Hamid Oughaddou 《Advanced functional materials》2021,31(7):2007013
Silicene, a new 2D material has attracted intense research because of the ubiquitous use of silicon in modern technology. However, producing free-standing silicene has proved to be a huge challenge. Until now, silicene could be synthesized only on metal surfaces where it naturally forms strong interactions with the metal substrate that modify its electronic properties. Here, the authors report the first experimental evidence of silicene nanoribbons on an insulating NaCl thin film. This work represents a major breakthrough, for the study of the intrinsic properties of silicene, and by extension to other 2D materials that have so far only been grown on metal surfaces. 相似文献
75.
Human error probability (HEP) evaluation and prediction is one of the most significant tasks to enhance human reliability in marine industry. Among various kinds of HEP evaluation techniques, the Human Error Assessment and Reduction Technique (HEART) technique is regarded as an effective and empirical tool that has been widely adopted in various fields. However, current HEART techniques are insufficient to address HEP evaluation problem in which the self-assurance of expert's judgment and inter-dependencies between Error-producing conditions (EPCs) are considered. Therefore, the purpose of this paper is to develop a hybrid HEART framework (H-HEART-F) to address this problem by integrating Z-numbers and the decision-making trial and evaluation laboratory (DEMATEL) method. First, the Z-numbers are introduced to model the uncertainty and self-assurance of evaluation information from various experts. Then, the Z-number power weighted average (Z-PWA) operator is proposed to aggregate the individual evaluation information into a group direct influenced matrix. Next, an extended DEMATEL method based on possibility degree measure is constructed to determine the proportion of effect of each EPC by considering the self-assurance of expert's judgment and inter-dependencies between EPCs. Finally, the HEP estimation for the cargo loading operation in oil or chemical tanker ship is presented to demonstrate the availability and feasibility of the H-HEART-F. After that, the sensitivity analysis and comparison study are conducted to further illustrate the reasonableness and effectiveness of the proposed method. 相似文献
76.
《Ceramics International》2021,47(19):27177-27187
BaZrO3-based materials doped with a trivalent cation have excellent chemical stability and relatively high proton conductivity which makes them potential proton conducting oxide materials for various electrochemical device applications such as hydrogen processing, high-temperature electrolysis, and solid electrolyte in fuel cells. However, BaZrO3 showed poor sinterability, requiring high sintering temperatures (1700–2100 °C) with longtime sintering (20–100 h) to achieve the desired microstructure and grain growth. This sintering problem can be solved by slightly doping BaZrO3 with a sintering aid element. Therefore, in this study, two different zirconate proton conductors: BaZr0·9Y0·1O3-α (BZY) and BaZr0·955Y0·03Co0·015O3-α (BZYC) were sintered in an air atmosphere and an oxygen atmosphere for 20 h in the temperature range of 1500–1640 °C. The sinterability was evaluated by analyzing the XRD diffraction patterns, lattice constant, lattice strain, crystallite size, relative density, open porosity, closed porosity, surface morphology, grain size, and grain boundary distribution, using the XRD, SEM, EDX, and Archimedes density measurement methods. It is concluded that in an oxygen atmosphere, sintering aid Co not only improves the relative density but also produces highly dense fine particles with clear grain boundaries which are promising for electrochemical hydrogen device applications. 相似文献
77.
Shi Pu Xingkai Yu Jianxun Li 《International Journal of Adaptive Control and Signal Processing》2021,35(8):1498-1512
This article considers a distributed Kalman filtering problem for linear system contaminated by complex multi-channel random uncertain parameter in which a number of nodes cooperative without central coordination to estimate a common state based on local measurements and data received from neighbors. We propose an approach to eliminate this error propagation. The proposed local filters are guaranteed to be stable under some mild conditions on certain global structural data, and their fusion yields the centralized Kalman estimate. Then, we extend this method to smoothing and deconvolution algorithm. Finally, simulation experiments demonstrate the validity of the proposed approach. 相似文献
78.
An electrolyte Equation of State is presented by combining the Cubic Plus Association Equation of State,Mean Spherical Approximation and the Born equation.This new model uses experimental relative static permittivity,intend to predict well the activity coefficients of individual ions (ACI) and liquid densities of aqueous solutions.This new model is applied to model water + NaCl binary system and water + gas +NaCl ternary systems.The cation/anion-water interaction parameters of are obtained by fitting the exper-imental data of ACI,mean ionic activity coefficients (MIAC) and liquid densities of water + NaCl binary system.The cation/anion-gas interaction parameters are obtained by fitting the experimental data of gas solubilities in aqueous NaCl solutions.The modeling results show that this new model can correlate well with the phase equilibrium and volumetric properties.Without gas,predictions for ACI,MIAC,and liquid densities present relative average deviations of 1.3%,3.6% and 1.4% compared to experimental ref-erence values.For most gas-containing systems,predictions for gas solubilities present relative average deviations lower than 7.0%.Further,the contributions of ACI,and salting effects of NaCl on gases are ana-lyzed and discussed. 相似文献
79.
In the electro-deoxidation process, carbon parasitic reaction (CO32- + 4e-=C + 3O2-) usually occurs when using carbon materials as the anode, which leads to increase of the carbon content in the final metal and decrease of the current efficiency of the process. The aim of this work is to reduce the negative effect of carbon parasitic reaction on the electrolysis process by adjusting anode current density. The results indicate that lower graphite anode area can achieve higher current density, which is helpful to increase the nucleation site of CO2 bubbles. Most of CO2 would be released from the anode instead of dissolution in the molten CaCl2 and reacting with O2- to form CO32-, thus decreasing the carbon parasitic reaction of the process. Furthermore, the results of the compared experiments show that when the anode area decreases from 172.78 to 4.99 cm2, CO2 concentration in the released gases increases significantly, the carbon mass content in the final metal product decreased from 1.09% to 0.13%, and the current efficiency increased from 6.65% to 36.50%. This study determined a suitable anode current density range for reducing carbon parasitic reaction and provides a valuable reference for the selection of the anode in the electrolysis process. 相似文献
80.
Nassim Razaaly Daan Crommelin Pietro Marco Congedo 《International journal for numerical methods in engineering》2020,121(9):2086-2105
This study considers an efficient method for the estimation of quantiles associated to very small levels of probability (up to O(10−9)), where the scalar performance function J is complex (eg, output of an expensive-to-run finite element model), under a probability measure that can be recast as a multivariate standard Gaussian law using an isoprobabilistic transformation. A surrogate-based approach (Gaussian Processes) combined with adaptive experimental designs allows to iteratively increase the accuracy of the surrogate while keeping the overall number of J evaluations low. Direct use of Monte-Carlo simulation even on the surrogate model being too expensive, the key idea consists in using an importance sampling method based on an isotropic-centered Gaussian with large standard deviation permitting a cheap estimation of small quantiles based on the surrogate model. Similar to AK-MCS as presented in the work of Schöbi et al., (2016), the surrogate is adaptively refined using a parallel infill criterion of an algorithm suitable for very small failure probability estimation. Additionally, a multi-quantile selection approach is developed, allowing to further exploit high-performance computing architectures. We illustrate the performances of the proposed method on several two to eight-dimensional cases. Accurate results are obtained with less than 100 evaluations of J on the considered benchmark cases. 相似文献