The palladium-catalyzed borylative cyclization via C—H activation has been developed.By this chemistry,the indole-fused dihydro-pyrrole motif,which is a kind of important unit in natural products and bio-active molec...The palladium-catalyzed borylative cyclization via C—H activation has been developed.By this chemistry,the indole-fused dihydro-pyrrole motif,which is a kind of important unit in natural products and bio-active molecules,could be constructed and installed with a boric ester group.Furthermore,the utilities of products have been illustrated by the study of further transformations.Importantly,by using chiral ligand,the enantioselectivity of this borylative cyclization reaction could be controlled.Moreover,the borylative mechanism,which should proceed through a Pd(II)/Pd(IV)catalytic cycle,has been proposed based on the DFT calculations.展开更多
Simultaneous monitoring of diverse salivary parameters can reveal underlying mechanisms of intraoral biological processes and offer profound insights into the evolution of oral diseases.However,conventional analytical...Simultaneous monitoring of diverse salivary parameters can reveal underlying mechanisms of intraoral biological processes and offer profound insights into the evolution of oral diseases.However,conventional analytical devices with bulky volumes,rigid formats,and discrete sensing mechanisms deviate from the requirements of continuous biophysiological quantification,resulting in huge difficulty in precise clinical diagnosis and pathogenetic study.Here,we present a flexible hybrid electronic system integrated with functional nanomaterials to continuously sense Ca^(2+),pH,and temperature for wireless real-time oral health monitoring.The miniaturized system with an island-bridge structure that is designed specifically to fit the teeth is only 0.4g in weight and 31.5×8.5×1.35 mm^(3) in dimension,allowing effective integration with customized dental braces and comfort attachment on teeth.Characterization results indicate high sensitivities of 30.3 and 60.6 mV/decade for Ca^(2+)and pH with low potential drifts.The system has been applied in clinical studies to conduct Ca^(2+)and pH mappings on carious teeth,biophysiological monitoring for up to 12 h,and outcome evaluation of dental restoration,providing quantitative data to assist in the diagnosis and understanding of oral diseases.Notably,caries risk assessment of 1o human subjects using the flexible system validates the important role of saliva buffering capacity in caries pathogenesis.The proposed flexible system may offer an open platform to carry diverse components to support both clinical diagnosis and treatment as well as fundamental researchfororaldiseases and induced systemicdiseases.展开更多
基金support is from Tianjin University,State Key Laboratory of Elemento-Organic Chemistry,and the National Natural Science Foundation of China(Nos.21801181,22073066,21503143 and 21975179).
文摘The palladium-catalyzed borylative cyclization via C—H activation has been developed.By this chemistry,the indole-fused dihydro-pyrrole motif,which is a kind of important unit in natural products and bio-active molecules,could be constructed and installed with a boric ester group.Furthermore,the utilities of products have been illustrated by the study of further transformations.Importantly,by using chiral ligand,the enantioselectivity of this borylative cyclization reaction could be controlled.Moreover,the borylative mechanism,which should proceed through a Pd(II)/Pd(IV)catalytic cycle,has been proposed based on the DFT calculations.
基金This work was supported by the Key Research and Develop-ment Program,of Zhejiang,Province,under_grant no.2021C05005the National Natural Science Foundationof China under grant no.52121002.
文摘Simultaneous monitoring of diverse salivary parameters can reveal underlying mechanisms of intraoral biological processes and offer profound insights into the evolution of oral diseases.However,conventional analytical devices with bulky volumes,rigid formats,and discrete sensing mechanisms deviate from the requirements of continuous biophysiological quantification,resulting in huge difficulty in precise clinical diagnosis and pathogenetic study.Here,we present a flexible hybrid electronic system integrated with functional nanomaterials to continuously sense Ca^(2+),pH,and temperature for wireless real-time oral health monitoring.The miniaturized system with an island-bridge structure that is designed specifically to fit the teeth is only 0.4g in weight and 31.5×8.5×1.35 mm^(3) in dimension,allowing effective integration with customized dental braces and comfort attachment on teeth.Characterization results indicate high sensitivities of 30.3 and 60.6 mV/decade for Ca^(2+)and pH with low potential drifts.The system has been applied in clinical studies to conduct Ca^(2+)and pH mappings on carious teeth,biophysiological monitoring for up to 12 h,and outcome evaluation of dental restoration,providing quantitative data to assist in the diagnosis and understanding of oral diseases.Notably,caries risk assessment of 1o human subjects using the flexible system validates the important role of saliva buffering capacity in caries pathogenesis.The proposed flexible system may offer an open platform to carry diverse components to support both clinical diagnosis and treatment as well as fundamental researchfororaldiseases and induced systemicdiseases.
