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Weiyi Li Geng Leng Caiqin Li Yajing Lyu 《International journal of quantum chemistry》2020,120(8):e26150
The mechanisms of CO2 coupling with the propargylic alcohol using alkali carbonates M2CO3 (M = Li, Na, K, Cs) have been investigated by means of density functional theory calculations. The calculations reveal that the target product tetronic acid (TA) is yielded through two stages: (a) the formation of the α-alkylidene cyclic carbonate (αACC) intermediate via Cs2CO3-mediated carboxylative cyclization of the propargylic alcohol with CO2, and (b) the conversion of the αACC intermediate with Cs2CO3 to produce the cesium salt of the TA. Since the overall kinetic barriers for the two stages are comparable and affordable, the excellent chemoselectivity to the TA should be primarily originated from the high thermodynamic stability of the cesium salt of the TA. Moreover, relative to the TA, the possibility to yield the by-product acyclic carbonate can be excluded due to the both kinetics and thermodynamic inferiority. This result is different from the organic base-mediated reaction. Alternatively, our calculations predict that CsHCO3 together generated with the cesium salt of the TA might also be an available mediating reagent for the incorporation of CO2 with the propargylic alcohol. Compared to other alkali carbonates M2CO3 (M = Li, Na, K), the stronger basicity of Cs2CO3 and the lower ionic potential of cesium ion can raise the effective concentration of the αACC intermediate, and thus the conversion of the αACC intermediate into the cesium salt of the TA can be achieved with high yield. 相似文献
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Su X. F. Zhang Y. L. Maximov A. L. Zhang K. Xin Q. Feng C. Q. Bai X. F. Wu W. 《Russian Journal of Applied Chemistry》2020,93(1):127-136
Russian Journal of Applied Chemistry - Nanoscale ZSM-5 (AlZ5-D) and Ga-substituted ZSM-5 zeolites ((Al,Ga)Z5-D and GaZ5-D) were synthesized by a green dry-gel conversion strategy. For comparison,... 相似文献
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Journal of Thermal Analysis and Calorimetry - In the present work, pyrolysis kinetic mechanism was studied for regenerated cellulosic fiber (RCF) and composite RCF containing silicon/nitrogen flame... 相似文献
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S. Q. Hou W. Wang Z. Y. Wang Z. W. Hu K. Liu 《Journal of Applied Mechanics and Technical Physics》2018,59(1):153-162
In order to investigate the characteristics of force chains in a granular flow system, a parallel plate shear cell is constructed to simulate the shear movement of an infinite parallel plate and observe variations in relevant parameters. The shear dilatancy process is divided into three stages, namely, plastic strain, macroscopic failure, and granular recombination. The stickslip phenomenon is highly connected with the evolution of force chains during the shear dilatancy process. The load–distribution rate curves and patterns of the force chains are utilized to describe the load-carrying behaviors and morphologic changes of force chains separately. Force chains, namely, “diagonal gridding,” “tadpole-shaped,” and “pinnate” are defined according to the form of the force chains in the corresponding three stages. 相似文献
6.
Ding Q. Yao M. Wu Sh. Zeng M. Xue N. Wu D. Xu J. 《Journal of Applied Spectroscopy》2022,89(4):712-718
Journal of Applied Spectroscopy - Based on partial least squares (PLS) analysis, the effects of different smoothing points and different preprocessing methods on the accuracy and precision of the... 相似文献
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Transport in Porous Media - The theme of coupling problems for adsorption, absorption and thermochemical transport in porous media is very important for engineering applications. Based on the... 相似文献
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Experimental Mechanics - Insufficient data are available to fully understand the effects of metal additive manufacturing (AM) defects for widespread adoption of the emerging technology.... 相似文献
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