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101.
Synthesis of multi‐functionalized carbonyl compounds by palladium–catalysed γ‐substitution of MBH adducts with activated amides 下载免费PDF全文
Gao Pei‐Sen Zhang Jin‐Lei Li Ning Zheng Zhan Jiang Yuan Yang Gao Zi‐Wei Zhang Weiqiang Xu Li‐Wen 《应用有机金属化学》2018,32(3)
Catalytic allylic γ‐substitution with Morita‐Baylis‐Hillman (MBH) adducts for creating a new family of unsymmetrical dicarbonyl compounds was presented in this work, in which a variety of allylated amide products were achieved in good yields and high regioselectivity with excellent linear‐to‐branched ratios. Especially, it was found that the Pd/HZNU‐Phos complex exhibited remarkably high activity (with a TON up to 16800) in this transformation between dicarbonyl amides and MBH adducts. In addition, the possibly multisite interaction between multifunctional Pd/HZNU‐Phos catalyst system and substrates might responsible for its exceptionally high efficiency in this reaction. 相似文献
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103.
Chain-like systems have been studied by many researchers for their simple structure and wide range of application. Previously, the damage in a chain-like system was detected by the reduction of the mass-normalized stiffness coefficient for certain elements as reported by Nayeri et al. (2008 [16]). However, some shortcomings exist in that approach and for overcoming them; an improved approach is derived and presented in this paper. In our improved approach, the mass normalized stiffness coefficients under two states (baseline state and potentially damaged state) are first estimated by a least square method, then these mass-stiffness coupled coefficients are decoupled to derive stiffness and mass relative change ratios for individual elements. These ratios are assembled in a vector, which is defined as damage indication vector (DIV). Each component in DIV is normalized individually to one to get multiple solutions. These solutions are averaged for estimating relative system changes, while abnormal solutions are discarded. The work of judging a solution as normal or abnormal is done by a cluster analysis algorithm. The most intriguing merit of this improved approach is that the relative stiffness and mass changes, which are coupled in the previous approach, can be separately identified. By this approach, the damage (single or multiple) extent and location can be correctly detected under operational conditions, meanwhile the proposed damage index has a clear physical meaning and is directly related to the stiffness reduction of corresponding structural elements. For illustrating the effectiveness and robustness of the improved approach, numerical simulation of a four floor building was carried out and experimental data from a structure tested at the Los Alamos National Laboratory was employed. Identified structural changes with both simulation and experimental data properly indicated the location and extent of actual structural damage, which validated the proposed approach. 相似文献
104.
Optimizing Optoelectronic Properties of Pyrimidine‐Based TADF Emitters by Changing the Substituent for Organic Light‐Emitting Diodes with External Quantum Efficiency Close to 25 % and Slow Efficiency Roll‐Off 下载免费PDF全文
Kailong Wu Tao Zhang Lisi Zhan Dr. Cheng Zhong Prof. Shaolong Gong Prof. Nan Jiang Prof. Zheng‐Hong Lu Prof. Chuluo Yang 《Chemistry (Weinheim an der Bergstrasse, Germany)》2016,22(31):10860-10866
A series of green butterfly‐shaped thermally activated delayed fluorescence (TADF) emitters, namely PXZPM , PXZMePM , and PXZPhPM , are developed by integrating an electron‐donor (D) phenoxazine unit and electron‐acceptor (A) 2‐substituted pyrimidine moiety into one molecule via a phenyl‐bridge π linkage to form a D –π–A–π–D configuration. Changing the substituent at pyrimidine unit in these emitters can finely tune their emissive characteristics, thermal properties, and energy gaps between the singlet and triplet states while maintaining frontier molecular orbital levels, and thereby optimizing their optoelectronic properties. Employing these TADF emitters results in a green fluorescent organic light‐emitting diode (OLED) that exhibits a peak forward‐viewing external quantum efficiency (EQE) close to 25 % and a slow efficiency roll‐off characteristic at high luminance. 相似文献
105.
Molecular‐level structures at poly(4‐vinyl pyridine)/acid interfaces probed by nonlinear vibrational spectroscopy 下载免费PDF全文
Mingcong Wang Bolin Li Zhan Chen Xiaolin Lu 《Journal of Polymer Science.Polymer Physics》2016,54(8):848-852
The molecular structures of the interfaces between a solid poly(4‐vinyl pyridine) (P4VP) surface and poly(acrylic acid) (PAA) as well as hydrochloric acid (HCl) solutions were probed using sum frequency generation (SFG) vibrational spectroscopy in situ in real time. Spectroscopic results clearly reveal that the PAA molecules are adsorbed onto the P4VP surface via hydrogen bonding at the P4VP/PAA solution interface while the P4VP surface is protonated at the P4VP/HCl solution interface. Consequently, the water molecules near the interfaces are strongly perturbed by these two interactions, exhibiting different orderings at the two interfaces. This work clearly demonstrates the power of studying the interfacial molecular‐level structures via nonlinear vibrational spectroscopy when molecular adsorption happens at the solid–liquid interface and paves a way for our future study on tracing the adsorption dynamics of polymer chains onto solid surfaces. © 2015 Wiley Periodicals, Inc. J. Polym. Sci., Part B: Polym. Phys. 2016 , 54, 848–852 相似文献
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107.
In this study, a solution to one-dimensional vertical airflow induced by the time-dependent atmospheric pressure fluctuations is developed in a three-layer unsaturated zone. The discrete atmospheric pressure data are transformed into a continuous boundary condition using the Fourier series analysis. The solution is applied to interpret the field air pressure data in a three-layer unsaturated zone reported in previous studies. The new solution improves the previous solution by reducing the required data measurement and input. The new solution is found to be accurate enough for the purpose of this study by comparing with a numerical solution developed in COMSOL Multiphysics. Given the necessary hydrogeological parameters, the new solution is capable of calculating the air permeability of each layer above a specified depth where the air pressures are known. Sensitivity analysis of the new solution shows that location, thickness, and air permeability of the less permeable layer impose large influence on the propagation of the atmospheric pressure fluctuations. Variations of air-filled porosity in soil layers in/below the less permeable layer may lead to greater amplitude attenuation and phase lag of air pressure than those in soil layers above the less permeable layer. 相似文献
108.
Bai‐Zhan Liu Li Yao Sai‐Jing Zheng Wei‐Miao Wang Xiao‐Lan Zhu Jun Yang 《中国化学会会志》2013,60(8):1055-1061
An efficient and sensitive analytical method based on molecularly imprinted solid‐phase extraction (MISPE) and reverse‐phase ultrasound‐assisted dispersive liquid–liquid microextraction (USA‐DLLME) coupled with LC–MS/MS detection was developed and validated for the analysis of urinary 4‐(methylnitrosamino)‐1‐(3‐pyridyl)‐1‐butanol (NNAL), a tobacco‐specific nitrosamine metabolite. The extraction performances of NNAL on three different solid‐phase extraction (SPE) sorbents including the hydrophilic‐lipophilic balanced sorbent HLB, the mixed mode cationic MCX sorbent and the molecularly imprinted polymers (MIP) sorbent were evaluated. Experimental results showed that the analyte was well retained with the highest extraction recovery and the optimum purification effect on MIP. Under the optimized conditions of MIP and USA‐DLLME, an enrichment factor of 23 was obtained. Good linearity relationship was obtained in the range of 5‐1200 pg/mL with a correlation coefficient of 0.9953. The limit of detection (LOD) was 0.35 pg/mL. The recoveries at three spiked levels ranged between 88.5% and 93.7%. Intra‐ and inter‐day relative standard deviations varied from 3.6% to 7.4% and from 5.4% to 9.7%, respectively. The developed method combing the advantages of MISPE and DLLME significantly improves the purification and enrichment of the analyte and can be used as an effective approach for the determination of ultra‐trace NNAL in complex biological matrices. 相似文献
109.
The internal redox esterification of α,β-unsaturated aldehydes and alcohols was carried out using different ionic liquids (ILs) as catalysts and reaction solvents. The basic ionic liquid, 1-butyl-3-methylimidazolium acetate ([bmim]OAc), exhibited the best activity for this reaction. The influences of the amount of ionic liquid catalyst and reaction time on yield of saturated ester have been investigated. The results showed that ionic liquid anions have a crucial effect on the redox esterification of α,β-unsaturated aldehydes and alcohols. The nucleophilic carbenes generated in situ from the ionic liquid cation were believed to be actual active species for this reactions. 相似文献
110.
The BiCl3‐catalyzed reaction of pyrroles with electron‐deficient olefins generated the corresponding Michael adducts in high yields. 相似文献