We report here a generic,green synthesis of 17 valuable syn-aryl-(2S,3R)-2–chloro-3–hydroxy esters(syn-(2S,3R)-1)in 73%-99%isolated yields along with 6.1:1–83:1 dr and 31%~>99%ee,through dynamic reductive kineti...We report here a generic,green synthesis of 17 valuable syn-aryl-(2S,3R)-2–chloro-3–hydroxy esters(syn-(2S,3R)-1)in 73%-99%isolated yields along with 6.1:1–83:1 dr and 31%~>99%ee,through dynamic reductive kinetic resolution of racemic arylα–chloroβ-keto esters(2)catalyzed by an engineered ketoreductase which was obtained via ep PCR-based directed evolution.The hectogram scale synthesis of syn-(2S,3R)-1b at a substrate concentration of 120 g/L showcased the application potential of the biocatalytic method developed presently.展开更多
The"solid-liquid"behavior of vitrimers have not been systematically investigated.Herein,a series of"solid-liquid"vitrimers bearing varying contents of dynamic boronic ester bonds were synthesized v...The"solid-liquid"behavior of vitrimers have not been systematically investigated.Herein,a series of"solid-liquid"vitrimers bearing varying contents of dynamic boronic ester bonds were synthesized via thiol-ene click reactions.These vitrimers allow for flexibile modulation of their network structures and thus show a range of intriguing properties including high stretchability,flexible transition from elasticity to plasticity,strong strain rate dependence,and solid-liquid performance.The dynamic association rate of boronic ester bonds within these vitrimers could be apparently accelerated via increasing the content of boronic ester,which could be used to shape-program the flat vitrimer films into various complex 3D structures just with external force.Materials with such versatile dynamic behavior may open up a range of new applications.展开更多
基金The National Key Research and Development Program of China(Nos.2021YFA0911400 and 2021YFF0600704)the National Natural Science Foundation of China(Nos.22071033 and 21801047)are acknowledged for the financial supports。
文摘We report here a generic,green synthesis of 17 valuable syn-aryl-(2S,3R)-2–chloro-3–hydroxy esters(syn-(2S,3R)-1)in 73%-99%isolated yields along with 6.1:1–83:1 dr and 31%~>99%ee,through dynamic reductive kinetic resolution of racemic arylα–chloroβ-keto esters(2)catalyzed by an engineered ketoreductase which was obtained via ep PCR-based directed evolution.The hectogram scale synthesis of syn-(2S,3R)-1b at a substrate concentration of 120 g/L showcased the application potential of the biocatalytic method developed presently.
基金supported by the National Natural Science Foundation of China(No.51973023)Sichuan Science and Technology Program(No.2021JDRC0014).
文摘The"solid-liquid"behavior of vitrimers have not been systematically investigated.Herein,a series of"solid-liquid"vitrimers bearing varying contents of dynamic boronic ester bonds were synthesized via thiol-ene click reactions.These vitrimers allow for flexibile modulation of their network structures and thus show a range of intriguing properties including high stretchability,flexible transition from elasticity to plasticity,strong strain rate dependence,and solid-liquid performance.The dynamic association rate of boronic ester bonds within these vitrimers could be apparently accelerated via increasing the content of boronic ester,which could be used to shape-program the flat vitrimer films into various complex 3D structures just with external force.Materials with such versatile dynamic behavior may open up a range of new applications.
基金supported by the National Natural Science Foundation of China(52172156,51832005)the Natural Science Foundation of Fujian Province of China(2023J06005)the Natural Science Foundation of Zhejiang Province(LD22E010001)。
