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61.
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
62.
By adopting a perturbation method and a local thermal nonequilibrium model, nonlinear thermal convection in an anisotropic porous layer saturated by an elasticoviscous fluid is investigated. An elasticoviscous fluid is modeled by a modified Darcy‐Oldroyd‐B model, and the fluid and solid phase temperatures are represented using a two‐field model for the heat transport equation. Anisotropy in permeability and fluid and solid thermal conductivities are considered. A cubic Landau equation is derived separately to study the stability of bifurcating solution of both stationary and oscillatory convection, and the results of linear instability theory are delineated. The boundary between stationary and oscillatory convection is demarcated by identifying codimension‐two points in the viscoelastic parameters plane. It is found that the subcritical instability is not possible, and the linear instability analysis itself completely captures the behavior of the onset of convection. Heat transfer is obtained in terms of Nusselt number, and the effect of governing parameters on the same is discussed. The results of the Maxwell fluid are obtained as a particular case from the present study. 相似文献
63.
64.
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
65.
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
66.
《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
67.
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
68.
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
69.
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
70.
Movement and distribution of Sitophilus zeamais adults and relationship between their trapping frequency and insect density were determined in one tonne wheat with 11.5 ± 0.2, 12.5 ± 0.1 and 13.5 ± 0.2% moisture contents (wet basis) inside cylindrical bins at 20, 25 and 30 °C. The introduced adult densities were 0.5, 1.0, and 2.0 adults/kg wheat (A/kg). Inside each bin, 15 probe traps were vertically installed in three layers. In each layer, five traps were installed at the center and half radii of the bin individually. The trapped adults were counted daily up to 7 d, and then 15 kg wheat was sampled at each trap location. The insect number in each sample was counted.The recovered adults in the top layer were less than that in the middle layer, while no significant difference between at middle and bottom layers. In each layer, adults preferred the center location at 0.5 A/kg, while this trend was unidentified at other densities. There was an autocorrelation of insect densities at adjacent locations at ≥ 1.0 A/kg, while no autocorrelation in the vertical direction. The adults had an aggregation distribution at any temperature, moisture content and adult density. The normal and Poisson model could not be used to describe the distribution of the count frequency of the adults in the samples, while the negative binomial model could describe this distribution in 18 out of 27 sampling sets at ≤ 1.0 A/kg. The trapping frequency was strongly influenced by the trapping period and increased with the increase of insect densities. The relationship between adult densities and trapping frequencies at the sampling locations had a significant difference at different grain temperatures, while no difference at different moisture contents, grain depths, and locations. 相似文献