In this article, series of novel bi-SOaH-functionalized ILs were synthesized using simple, efficient and economic procedure. Hammer method had been used to determine the acidity order of these ionic liquids, and the a...In this article, series of novel bi-SOaH-functionalized ILs were synthesized using simple, efficient and economic procedure. Hammer method had been used to determine the acidity order of these ionic liquids, and the acidifies of bi-SOaH-functionalized ILs were stronger than that of traditional single-SOaH-functionalized ILs. Their catalytic activities in the synthesis of N-（3-phenyl）-3- oxo-1-（phenylpropyl）acetamide were investigated and they were consistent with their acidities.展开更多
In this article,an efficient,simple and environmentally friendly approach to the synthesis of diacetals(diketals)pentaerythritol using SOH-functionalized ionic liquids(ILs)as catalysts was reported.The ILs show high c...In this article,an efficient,simple and environmentally friendly approach to the synthesis of diacetals(diketals)pentaerythritol using SOH-functionalized ionic liquids(ILs)as catalysts was reported.The ILs show high catalytic activity and reusability with good to excellent yields of the desired products.Hammett method has been used to determine the acidity order of these ionic liquids and the results are consistent with the catalytic activities observed in acetalization reaction.Maximum product yield of 93%was observed on using[PSPy][OTf]as catalyst and it can be reused at least 8 times without obvious activity loss.展开更多
A meticulous design of the local environment at the interface between active species and the support,aimed at optimizing the adsorption of H_(2)O molecules and BH_(4)^(-)anion,offers an ideal strategy for enhancing hy...A meticulous design of the local environment at the interface between active species and the support,aimed at optimizing the adsorption of H_(2)O molecules and BH_(4)^(-)anion,offers an ideal strategy for enhancing hydrogen generation via Na BH4hydrolysis through dual activation pathways.Theoretical predictions based on d-band center analysis and electron transfer calculations suggest that introducing-OH functional groups induce charge redistribution,enhancing charge concentration on alk-Ti_(3)C_(2)and facilitating the adsorption and activation of dual active species,H2O molecules and BH4-anion.Inspired by these predictions,the optimized alk-Ti_(3)C_(2)/Ru Oxcatalyst demonstrates the highest catalytic activity,achieving a hydrogen generation rate(HGR)of 9468 m L min^(-1)gcat.^(-1).Both experimental data and theoretical analyses confirm that the-OH functional groups promote charge enrichment on alk-Ti_(3)C_(2),optimizing the adsorption of H_(2)O molecules and BH_(4)^(-)anion,and reducing the dissociation energy barrier of the*OH–H-TS intermediate.This dual activation pathways mechanism lowers the activation energy for Na BH4hydrolysis,significantly enhancing the HGR performance.These findings,guided by theoretical insights,establish alk-Ti_(3)C_(2)/Ru Oxas an efficient catalyst for Na BH4hydrolysis and provide a strong foundation for future hydrogen generation catalyst designs.展开更多
基金the National Natural Science Foundation ofChina(Nos.21003049,21073064)the Fundamental Research Funds for the Central Universities for financial support
文摘In this article, series of novel bi-SOaH-functionalized ILs were synthesized using simple, efficient and economic procedure. Hammer method had been used to determine the acidity order of these ionic liquids, and the acidifies of bi-SOaH-functionalized ILs were stronger than that of traditional single-SOaH-functionalized ILs. Their catalytic activities in the synthesis of N-（3-phenyl）-3- oxo-1-（phenylpropyl）acetamide were investigated and they were consistent with their acidities.
基金supported by National 863 High-Tech Research and Development Program of China(No. 2007AA05Z101)
文摘In this article,an efficient,simple and environmentally friendly approach to the synthesis of diacetals(diketals)pentaerythritol using SOH-functionalized ionic liquids(ILs)as catalysts was reported.The ILs show high catalytic activity and reusability with good to excellent yields of the desired products.Hammett method has been used to determine the acidity order of these ionic liquids and the results are consistent with the catalytic activities observed in acetalization reaction.Maximum product yield of 93%was observed on using[PSPy][OTf]as catalyst and it can be reused at least 8 times without obvious activity loss.
基金supported by the Hebei province Natural Science Foundation(No.B2023108012)the Science Research Project of Hebei Education Department(No.BJK2024137)+2 种基金the S&T Program of Xingtai(No.2023ZZ096)the National Natural Science Foundation of China(No.62004143)the Key R&D Program of Hubei Province(No.2022BAA084)。
文摘A meticulous design of the local environment at the interface between active species and the support,aimed at optimizing the adsorption of H_(2)O molecules and BH_(4)^(-)anion,offers an ideal strategy for enhancing hydrogen generation via Na BH4hydrolysis through dual activation pathways.Theoretical predictions based on d-band center analysis and electron transfer calculations suggest that introducing-OH functional groups induce charge redistribution,enhancing charge concentration on alk-Ti_(3)C_(2)and facilitating the adsorption and activation of dual active species,H2O molecules and BH4-anion.Inspired by these predictions,the optimized alk-Ti_(3)C_(2)/Ru Oxcatalyst demonstrates the highest catalytic activity,achieving a hydrogen generation rate(HGR)of 9468 m L min^(-1)gcat.^(-1).Both experimental data and theoretical analyses confirm that the-OH functional groups promote charge enrichment on alk-Ti_(3)C_(2),optimizing the adsorption of H_(2)O molecules and BH_(4)^(-)anion,and reducing the dissociation energy barrier of the*OH–H-TS intermediate.This dual activation pathways mechanism lowers the activation energy for Na BH4hydrolysis,significantly enhancing the HGR performance.These findings,guided by theoretical insights,establish alk-Ti_(3)C_(2)/Ru Oxas an efficient catalyst for Na BH4hydrolysis and provide a strong foundation for future hydrogen generation catalyst designs.
