A series of 2 (E) (4 hydroxy 3 methoxybenzylidene) 5 (N substituted ami nomethyl) cyclopentanones was synthesized and evaluated for the anti inflammatory activity. All of the target compounds were confirmed ...A series of 2 (E) (4 hydroxy 3 methoxybenzylidene) 5 (N substituted ami nomethyl) cyclopentanones was synthesized and evaluated for the anti inflammatory activity. All of the target compounds were confirmed by spectral analysis and elemental analysis. Preliminary pharmacological tests showed that several compounds exerted appreciable inhibitory effect on xylene induced ear edema in mice and that alteration of the substituents of anilines had significant influence in anti inflammatory potency.展开更多
A Michael addition is usually taken as a base-catalysed reaction. However, our synthesized 2-（quinolin-2-ylmethylene） malonic acid （QMA） as a Michael-type thiol fluorescent probe is acid-active in its sensing reac...A Michael addition is usually taken as a base-catalysed reaction. However, our synthesized 2-（quinolin-2-ylmethylene） malonic acid （QMA） as a Michael-type thiol fluorescent probe is acid-active in its sensing reaction. In this work, based on theoretic calculation and experimental study on 7-hydroxy-2-（quinolin-2-ylmethylene） malonic acid, we demonstrated that QMA as a Michael acceptor is acid-activatable, i.e., it works only in solutions at pH〈7, and the lower the pH of solutions is, the higher reactivity QMA has. In alkaline solution, the malonate QMA[-2H＋]2- cannot react with both RSand RSH. In contrast, 2-（quinolin-2- ylmethylene） malonic ester （QME）, the ester of QMA, reveal a contrary pH effect on its sensing reaction, that is, it can sense thiols in alkaline solutions but not in acidic solutions, like a normal base-catalysed Michael addition. The values of activation enthalpies from theoretic calculation support the above sensing behavior of two probes under different pH conditions. In acidic solutions, the protonated QMA is more highly reactive towards electrophilic attack over its other ionized states in neutral and alkaline solutions, and so can react with lowly reactive RSH. In contrast, there is a big energy barrier in the interaction of QME with RSH （acidic solutions）, and the reaction of QME with the highly reactive nucleophile RS- is a low activation energy process （in alkaline solutions）. Theoretic calculation reveals that the sensing reaction of QMA undergoes a 1,4-addition process with neutral thiols （RSH）, and a 1,2-addition pathway for the sensing reaction of QME with RS-. Therefore, the sensing reaction of QMA is an acid-catalysed Michael addition via a 1,4-addition, and a normal base-catalysed Michael addition via a 1,2-addition.展开更多
This paper studies the reaction between alkaline metal ions Li＋, Na＋ and K＋ and ASR （alkali-silica reaction） reactive aggregates to determine whether Li＋ can substitute Na＋ and K＋ that are unified in cement pa...This paper studies the reaction between alkaline metal ions Li＋, Na＋ and K＋ and ASR （alkali-silica reaction） reactive aggregates to determine whether Li＋ can substitute Na＋ and K＋ that are unified in cement paste. Reactive aggregates use meta-sandstone from eastern Taiwan and Pyrex glass. Non-reactive aggregates use siliceous sand. The results show that the dissolved amount of SiO2 is lower when the reactive aggregates are immersed in an 80 ℃1 N LiOH＇H20 solution than in NaOH and KOH solutions. The reduced amounts of OH and Li＋ in the solution are also higher than those in the NaOH and KOH solutions. These results reveal that reactive SiO2 can react with LiOH to form a reactant with low water solubility. When the powder of the cement paste is immersed in an 80 ℃ 1 N LiOH-H2O solution, the amounts of free Na＋ and K＋ in the solution are higher than those in water. The increased amount increases with the duration of immersion. The amount of Li＋ in the solution also decreases with the duration of immersion. These results reveal that Li＋ can substitute Na＋ and K＋ that are unified in cement paste, which indicates that ASR can be prevented with the existence of Li＋.展开更多
Ir-based dectrocatalysts have been system- atically studied for a variety of applications, among which the electrocatalysis for oxygen evolution reaction （OER） is one of the most prominent. The investigation on surf...Ir-based dectrocatalysts have been system- atically studied for a variety of applications, among which the electrocatalysis for oxygen evolution reaction （OER） is one of the most prominent. The investigation on surface-micro- structure-sensitive catalytic activity in different pH media is of great significance for developing efficient electrocatalysts and corresponding mechanism research. Herein, shape-tunable Ir- Pd alloy nanocrystals, including nano-hollow-spheres （NHSs）, nanowires （NWs）, and nanotetrahedrons （NTs）, are synthe- sized via a facile one-pot solvothermal method, Electro- chemical studies show that the OER activity of the Ir-Pd alloy nanocatalysts exhibits surface-microstructure-sensitive en- hancement in acidic and alkaline media. Ir-Pd NWs and NTs show more than five times higher mass activity than com- mercial Ir/C catalyst at an overpotential of 0.25 V in acidic and alkaline media. Post-XPS analyses reveal that surface Ir（VI） oxide generated at surface defective sites of Ir-Pd nanocata- lysts is a possible key intermediate for OER. In acidic medium, the specific activity of Ir-Pd nanocatalysts has a positive cor- relation with the surface roughness of NWs 〉 NHSs 〉 NTs. However, the strong dissociation of surface Ir（VI） species （IrO42-） at surface defective sites is a possible obstacle for the formation of Ir（VI） oxide, which reverses the activity sequence for OER in alkaline medium.展开更多
A highly porous nickel-film electrode with satisfactory mechanical strength was prepared by a facile vertical template-assisted composite electrodeposition method using polystyrene(PS) microspheres templates, with the...A highly porous nickel-film electrode with satisfactory mechanical strength was prepared by a facile vertical template-assisted composite electrodeposition method using polystyrene(PS) microspheres templates, with the aim of improving the electrocatalytic activity for the hydrogen-evolution reaction(HER). During the composite electrodeposition process, the hydrophobic PS microspheres were highly dispersed in the electrolyte with the help of a surfactant, and then co-deposited with Ni to form the film electrode. After removing the PS templates by annealing, a porous Ni film containing large amount of uniformly dispersed pores with narrow size distribution was obtained, and then applied as the electrode for the HER in an alkaline medium. As evidenced by the electrochemical analysis, the porous Ni film electrode exhibits higher catalytic activity as compared to a dense Ni film electrode and is superior to a Ni/Ru O2/Ce O2 commercial electrode. The effect of temperature on the catalytic properties of the porous Ni film electrode was also investigated; the activation energy was calculated as 17.26 k J/mol. The enhanced activity toward the HER was attributed to the improved electrochemical surface area and mass transportation facilitated by the high porosity of the synthesized Ni film electrode.展开更多
An efficient synthesis of chromeno[4,3-b]quinoline derivatives via one-pot,four-component reaction of 4-hydroxycoumarin, formaldehyde,cyclohexanedione,ammonium ceric nitrate under microwave irradiation was accomplishe...An efficient synthesis of chromeno[4,3-b]quinoline derivatives via one-pot,four-component reaction of 4-hydroxycoumarin, formaldehyde,cyclohexanedione,ammonium ceric nitrate under microwave irradiation was accomplished.The structures of these compounds were unambiguously confirmed by single crystal X-ray diffraction.Furthermore,the anti-AChE activities of these compounds in vitro were investigated at concentrations of 20μM and 50μM by using a standard Ellman's method.The relationship of inhibitory activities and structures of these chromeno [4,3-b]quinolines was also systematically studied.Of all the compounds investigated,4ag emerged as the most potent AChE inhibitor with IC50 values of 5.63μM,and it might be used as potent lead for the development anti-AChE agents.Moreover,molecular modelling was conducted to understand the optimal interaction of AChE with these types of compounds.展开更多
文摘A series of 2 (E) (4 hydroxy 3 methoxybenzylidene) 5 (N substituted ami nomethyl) cyclopentanones was synthesized and evaluated for the anti inflammatory activity. All of the target compounds were confirmed by spectral analysis and elemental analysis. Preliminary pharmacological tests showed that several compounds exerted appreciable inhibitory effect on xylene induced ear edema in mice and that alteration of the substituents of anilines had significant influence in anti inflammatory potency.
基金This work is supported by the National Natural Science Foundation of China （No.21272224）, the Open Research Fund of State Key Laboratory of Physical Chemistry of Solid Surfaces, Xiamen University （No.201410）, and the Open Research Fund of Key Laboratory of Advanced Scientific Computation, Xihua University （No.szjj2013-024）.
文摘A Michael addition is usually taken as a base-catalysed reaction. However, our synthesized 2-（quinolin-2-ylmethylene） malonic acid （QMA） as a Michael-type thiol fluorescent probe is acid-active in its sensing reaction. In this work, based on theoretic calculation and experimental study on 7-hydroxy-2-（quinolin-2-ylmethylene） malonic acid, we demonstrated that QMA as a Michael acceptor is acid-activatable, i.e., it works only in solutions at pH〈7, and the lower the pH of solutions is, the higher reactivity QMA has. In alkaline solution, the malonate QMA[-2H＋]2- cannot react with both RSand RSH. In contrast, 2-（quinolin-2- ylmethylene） malonic ester （QME）, the ester of QMA, reveal a contrary pH effect on its sensing reaction, that is, it can sense thiols in alkaline solutions but not in acidic solutions, like a normal base-catalysed Michael addition. The values of activation enthalpies from theoretic calculation support the above sensing behavior of two probes under different pH conditions. In acidic solutions, the protonated QMA is more highly reactive towards electrophilic attack over its other ionized states in neutral and alkaline solutions, and so can react with lowly reactive RSH. In contrast, there is a big energy barrier in the interaction of QME with RSH （acidic solutions）, and the reaction of QME with the highly reactive nucleophile RS- is a low activation energy process （in alkaline solutions）. Theoretic calculation reveals that the sensing reaction of QMA undergoes a 1,4-addition process with neutral thiols （RSH）, and a 1,2-addition pathway for the sensing reaction of QME with RS-. Therefore, the sensing reaction of QMA is an acid-catalysed Michael addition via a 1,4-addition, and a normal base-catalysed Michael addition via a 1,2-addition.
文摘This paper studies the reaction between alkaline metal ions Li＋, Na＋ and K＋ and ASR （alkali-silica reaction） reactive aggregates to determine whether Li＋ can substitute Na＋ and K＋ that are unified in cement paste. Reactive aggregates use meta-sandstone from eastern Taiwan and Pyrex glass. Non-reactive aggregates use siliceous sand. The results show that the dissolved amount of SiO2 is lower when the reactive aggregates are immersed in an 80 ℃1 N LiOH＇H20 solution than in NaOH and KOH solutions. The reduced amounts of OH and Li＋ in the solution are also higher than those in the NaOH and KOH solutions. These results reveal that reactive SiO2 can react with LiOH to form a reactant with low water solubility. When the powder of the cement paste is immersed in an 80 ℃ 1 N LiOH-H2O solution, the amounts of free Na＋ and K＋ in the solution are higher than those in water. The increased amount increases with the duration of immersion. The amount of Li＋ in the solution also decreases with the duration of immersion. These results reveal that Li＋ can substitute Na＋ and K＋ that are unified in cement paste, which indicates that ASR can be prevented with the existence of Li＋.
基金supported by the National Natural Science Foundation of China (21573005, 21771009 and 21621061)the National Key Research and Development Program (2016YFB0701100)Beijing Natural Science Foundation (2162019)
文摘Ir-based dectrocatalysts have been system- atically studied for a variety of applications, among which the electrocatalysis for oxygen evolution reaction （OER） is one of the most prominent. The investigation on surface-micro- structure-sensitive catalytic activity in different pH media is of great significance for developing efficient electrocatalysts and corresponding mechanism research. Herein, shape-tunable Ir- Pd alloy nanocrystals, including nano-hollow-spheres （NHSs）, nanowires （NWs）, and nanotetrahedrons （NTs）, are synthe- sized via a facile one-pot solvothermal method, Electro- chemical studies show that the OER activity of the Ir-Pd alloy nanocatalysts exhibits surface-microstructure-sensitive en- hancement in acidic and alkaline media. Ir-Pd NWs and NTs show more than five times higher mass activity than com- mercial Ir/C catalyst at an overpotential of 0.25 V in acidic and alkaline media. Post-XPS analyses reveal that surface Ir（VI） oxide generated at surface defective sites of Ir-Pd nanocata- lysts is a possible key intermediate for OER. In acidic medium, the specific activity of Ir-Pd nanocatalysts has a positive cor- relation with the surface roughness of NWs 〉 NHSs 〉 NTs. However, the strong dissociation of surface Ir（VI） species （IrO42-） at surface defective sites is a possible obstacle for the formation of Ir（VI） oxide, which reverses the activity sequence for OER in alkaline medium.
基金supported by the National Natural Science Foundation of China(51125007)the National Key Technology R&D Program of China(2009BAE87B00)
文摘A highly porous nickel-film electrode with satisfactory mechanical strength was prepared by a facile vertical template-assisted composite electrodeposition method using polystyrene(PS) microspheres templates, with the aim of improving the electrocatalytic activity for the hydrogen-evolution reaction(HER). During the composite electrodeposition process, the hydrophobic PS microspheres were highly dispersed in the electrolyte with the help of a surfactant, and then co-deposited with Ni to form the film electrode. After removing the PS templates by annealing, a porous Ni film containing large amount of uniformly dispersed pores with narrow size distribution was obtained, and then applied as the electrode for the HER in an alkaline medium. As evidenced by the electrochemical analysis, the porous Ni film electrode exhibits higher catalytic activity as compared to a dense Ni film electrode and is superior to a Ni/Ru O2/Ce O2 commercial electrode. The effect of temperature on the catalytic properties of the porous Ni film electrode was also investigated; the activation energy was calculated as 17.26 k J/mol. The enhanced activity toward the HER was attributed to the improved electrochemical surface area and mass transportation facilitated by the high porosity of the synthesized Ni film electrode.
基金NSFC(Grant No.81773557,81573279,81373255)Major Project of Technology Innovation Program of Hubei Province(Grant No.2016ACA126)+1 种基金NSFHP(Grant No.2017CFA024)and the Fun damental Research Funds for the Central Universities of China(Grant No.2042017kf0288)
文摘An efficient synthesis of chromeno[4,3-b]quinoline derivatives via one-pot,four-component reaction of 4-hydroxycoumarin, formaldehyde,cyclohexanedione,ammonium ceric nitrate under microwave irradiation was accomplished.The structures of these compounds were unambiguously confirmed by single crystal X-ray diffraction.Furthermore,the anti-AChE activities of these compounds in vitro were investigated at concentrations of 20μM and 50μM by using a standard Ellman's method.The relationship of inhibitory activities and structures of these chromeno [4,3-b]quinolines was also systematically studied.Of all the compounds investigated,4ag emerged as the most potent AChE inhibitor with IC50 values of 5.63μM,and it might be used as potent lead for the development anti-AChE agents.Moreover,molecular modelling was conducted to understand the optimal interaction of AChE with these types of compounds.
