Skeletal editing has emerged as a powerful tool in organic chemistry,enabling the simplification of synthetic routes to complex molecules[1].Indoles,electron-rich nitrogen-containing building blocks,represent privileg...Skeletal editing has emerged as a powerful tool in organic chemistry,enabling the simplification of synthetic routes to complex molecules[1].Indoles,electron-rich nitrogen-containing building blocks,represent privileged scaffolds prevalent in pharmaceuticals,natural products,and bioactive compounds.The application of skeletal editing strategies to modify such structures is highly valuable and in growing demand.Leveraging the electronrich nature of indoles at C2 and C3,single-carbon atom insertion using cationic carbyne equivalents offers an efficient approach for indole ring expansion to quinoline(Scheme 1a).However,existing methods predominantly rely on halocarbene precursors,which restricts the functional groups of ring-expanded products to halogen[2],alkyl,aryl,heteroaryl and ester moieties[3].This limitation hinders their utility in late-stage skeletal modifications of complex targets.展开更多
It is vital to develop efficient catalysts for desulfurization in fuels,reducing the pollution caused by sulfur oxides.In this study,polyoxometalate-based ionic liquid supported three-dimensionally ordered macroporous...It is vital to develop efficient catalysts for desulfurization in fuels,reducing the pollution caused by sulfur oxides.In this study,polyoxometalate-based ionic liquid supported three-dimensionally ordered macroporous silica(IL-3DOM SiO_(2))was successfully prepared for heterogeneous oxidative desulfurization of aromatic sulfur compounds.The as-prepared material was characterized using FTIR,XRD,XPS,SEM,TEM,and BET analysis,exhibiting a large pore size and a high specific surface area.The hybrid material with a 3DOM structure exhibited excellent desulfurization performance on aromatic sulfur compounds under mild conditions.Furthermore,no obvious decrease in activity was observed after seventeen cycles,revealing a good stability of the hybrid material.The as-prepared IL-3DOM SiO_(2) is an ideal candidate for applications in the future desulfurization industry.展开更多
Desulfurization in fuel has become more and more important due to increasingly stringent environmental protection policies.Mesoporous materials have attracted considerable attention owing to their excellent abilities ...Desulfurization in fuel has become more and more important due to increasingly stringent environmental protection policies.Mesoporous materials have attracted considerable attention owing to their excellent abilities in various catalytic reactions.Herein,we report the synthesis of molybdenum-containing dendritic mesoporous silica spheres via a facile Stöber approach and employ them in the removal of organic sulfur compounds.The dendritic mesoporous silica spheres not only provide a large specific surface area and pore volume but also possess a high dispersion of molybdenum species.Under optimal conditions,sulfur removal of the refractory aromatic sulfur compound 4,6-DMDBT can reach 100%in 40 minutes with a low dosage of oxidant.The catalysts can be reused nine times without a significant decrease.Furthermore,an oxidative desulfurization process was proposed through gas chromatography-mass spectrometry(GC-MS)analysis.展开更多
An interactive web tool,PredPotS,has been developed for predicting one-electron standard reduction potentials of organic molecules in aqueous solutions.The predictions are generated using deep learning models trained ...An interactive web tool,PredPotS,has been developed for predicting one-electron standard reduction potentials of organic molecules in aqueous solutions.The predictions are generated using deep learning models trained and validated on a chemically diverse database comprising reduction potentials of approximately 8000 organic compounds.The reduction potentials of this database were computed using a composite computational protocol that combines the semiempirical quantum chemical method(GFN2-xTB)and awell-established DFT approach(M06-2X functional along with the SMD solvent model).While this computational approach is cost-effective,it is subject to certain limitations,which are nonetheless duly accounted for in the development of the database.The applied graph-based deep learning methods perform remarkably well in terms of the standard performance metrics.By entering or uploading the SMILES codes of the molecules,PredPotS provides fast and sensible predictions for one-electron standard reduction potentials for a diverse set of organic molecules also in the range compatible with the electrochemical stability of aqueous electrolytes.The PredPotS web tool is particularly well-suited for screening redox-active candidates for aqueous organic redox flow batteries,but it may also prove useful in a variety of other electrochemical applications.展开更多
文摘Skeletal editing has emerged as a powerful tool in organic chemistry,enabling the simplification of synthetic routes to complex molecules[1].Indoles,electron-rich nitrogen-containing building blocks,represent privileged scaffolds prevalent in pharmaceuticals,natural products,and bioactive compounds.The application of skeletal editing strategies to modify such structures is highly valuable and in growing demand.Leveraging the electronrich nature of indoles at C2 and C3,single-carbon atom insertion using cationic carbyne equivalents offers an efficient approach for indole ring expansion to quinoline(Scheme 1a).However,existing methods predominantly rely on halocarbene precursors,which restricts the functional groups of ring-expanded products to halogen[2],alkyl,aryl,heteroaryl and ester moieties[3].This limitation hinders their utility in late-stage skeletal modifications of complex targets.
基金supported by the National Nature Science Foundation of China(No.21776116,21406092,and 21722604)the National Science and Technology Program(2017YFB0306*04-1*)+2 种基金the Postdoctoral Foundation of China(No.2017M621646)Advanced Talents of Jiangsu University(No.13JDG080)a project funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD).
文摘It is vital to develop efficient catalysts for desulfurization in fuels,reducing the pollution caused by sulfur oxides.In this study,polyoxometalate-based ionic liquid supported three-dimensionally ordered macroporous silica(IL-3DOM SiO_(2))was successfully prepared for heterogeneous oxidative desulfurization of aromatic sulfur compounds.The as-prepared material was characterized using FTIR,XRD,XPS,SEM,TEM,and BET analysis,exhibiting a large pore size and a high specific surface area.The hybrid material with a 3DOM structure exhibited excellent desulfurization performance on aromatic sulfur compounds under mild conditions.Furthermore,no obvious decrease in activity was observed after seventeen cycles,revealing a good stability of the hybrid material.The as-prepared IL-3DOM SiO_(2) is an ideal candidate for applications in the future desulfurization industry.
基金supported by the National Nature Science Foundation of China(No.21776116,21406092,21722604)Postdoctoral Foundation of China(No.2017M621646)+2 种基金Postdoctoral Foundation of Jiangsu Province(No.2018K083C)High-tech Research Key laboratory of Zhenjiang(SS_(2)018002)A Project Funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD).
文摘Desulfurization in fuel has become more and more important due to increasingly stringent environmental protection policies.Mesoporous materials have attracted considerable attention owing to their excellent abilities in various catalytic reactions.Herein,we report the synthesis of molybdenum-containing dendritic mesoporous silica spheres via a facile Stöber approach and employ them in the removal of organic sulfur compounds.The dendritic mesoporous silica spheres not only provide a large specific surface area and pore volume but also possess a high dispersion of molybdenum species.Under optimal conditions,sulfur removal of the refractory aromatic sulfur compound 4,6-DMDBT can reach 100%in 40 minutes with a low dosage of oxidant.The catalysts can be reused nine times without a significant decrease.Furthermore,an oxidative desulfurization process was proposed through gas chromatography-mass spectrometry(GC-MS)analysis.
基金funded by the European Union’s Horizon 2020 research and innovation programme under grant agreement No 875565 (CompBat project).
文摘An interactive web tool,PredPotS,has been developed for predicting one-electron standard reduction potentials of organic molecules in aqueous solutions.The predictions are generated using deep learning models trained and validated on a chemically diverse database comprising reduction potentials of approximately 8000 organic compounds.The reduction potentials of this database were computed using a composite computational protocol that combines the semiempirical quantum chemical method(GFN2-xTB)and awell-established DFT approach(M06-2X functional along with the SMD solvent model).While this computational approach is cost-effective,it is subject to certain limitations,which are nonetheless duly accounted for in the development of the database.The applied graph-based deep learning methods perform remarkably well in terms of the standard performance metrics.By entering or uploading the SMILES codes of the molecules,PredPotS provides fast and sensible predictions for one-electron standard reduction potentials for a diverse set of organic molecules also in the range compatible with the electrochemical stability of aqueous electrolytes.The PredPotS web tool is particularly well-suited for screening redox-active candidates for aqueous organic redox flow batteries,but it may also prove useful in a variety of other electrochemical applications.
