A metal-free cross coupling between common CH2Cl2 and carboxylic acids has been achieved with K2CO3 as the sole additive. This simple protocol is a convenient and cost-effective route to synthesize methylene diesters ...A metal-free cross coupling between common CH2Cl2 and carboxylic acids has been achieved with K2CO3 as the sole additive. This simple protocol is a convenient and cost-effective route to synthesize methylene diesters from a wide scope of carboxylic acids substrates with good functional group tolerance. Several gram-scale reactions have been performed to evaluate the effectiveness and practicality of this protocol.展开更多
A C/D ring synthon of vitamin D is readily obtained from cholesteryl acetate via oxidation, elimination of acetoxy group and Norrish type II photochemical reaction.
An efficient synthesis of functionalized 6-decalone 16, starting from a dienolate anion 3a via a tandem Michael reaction, is described. 16 could be used as a potential intermediate for synthesis of drimane related ses...An efficient synthesis of functionalized 6-decalone 16, starting from a dienolate anion 3a via a tandem Michael reaction, is described. 16 could be used as a potential intermediate for synthesis of drimane related sesquiterpenes.展开更多
This essay discusses some preliminary thoughts on the development of a rational and modular approach for molecular design in soft matter engineering and proposes ideas of structural and functional synthons for advance...This essay discusses some preliminary thoughts on the development of a rational and modular approach for molecular design in soft matter engineering and proposes ideas of structural and functional synthons for advanced functional materials. It echoes the Materials Genome Initiative by practicing a tentative retro-functional analysis （RFA） scheme. The importance of hierarchical structures in transferring and amplifying molecular functions into macroscopic properties is recognized and emphasized. According to the role of molecular segments in final materials, there are two types of building blocks： structural synthon and functional synthon. Guided by a specific structure for a desired function, these synthons can be modularly combined in various ways to construct molecular scaffolds. Detailed molecular structures are then deduced, designed and synthesized precisely and modularly. While the assembled structure and property may deviate from the original design, the study may allow further refinement of the molecular design toward the target function, The strategy has been used in the development of soft fullerene materials and other giant molecules. There are a few aspects that are not yet well addressed： （1） function and structure are not fully decoupled and （2） the assembled hierarchical structures are sensitive to secondary interactions and molecular geometries across different length scales. Nevertheless, the RFA approach provides a starting point and an alternative thinking pathway by provoking creativity with considerations from both chemistry and physics. This is particularly useful for engineering soft matters with supramolecular lattice formation, as in giant molecules, where the synthons are relatively independent of each other.展开更多
基金Financial support from the National Natural Science Foundation of China(NSFC, Nos. 21761021 and 21571094)Natural Science Foundation of Jiangxi Province(No. 20171BAB203002)Sci & Tech Project of Education Department of Jiangxi Province(No. 60007)
文摘A metal-free cross coupling between common CH2Cl2 and carboxylic acids has been achieved with K2CO3 as the sole additive. This simple protocol is a convenient and cost-effective route to synthesize methylene diesters from a wide scope of carboxylic acids substrates with good functional group tolerance. Several gram-scale reactions have been performed to evaluate the effectiveness and practicality of this protocol.
文摘A C/D ring synthon of vitamin D is readily obtained from cholesteryl acetate via oxidation, elimination of acetoxy group and Norrish type II photochemical reaction.
文摘An efficient synthesis of functionalized 6-decalone 16, starting from a dienolate anion 3a via a tandem Michael reaction, is described. 16 could be used as a potential intermediate for synthesis of drimane related sesquiterpenes.
基金financially supported by the 863 Program(No.2015AA020941)the National Natural Science Foundation of China(Nos.21474003 and 91427304)+1 种基金National Science Foundation of USA(Nos.DMR-0906898 and DMR-1408872)the Joint-Hope Education Foundation.W.B.Z.acknowledges support from the National"1000 Plan(Youth)"of China
文摘This essay discusses some preliminary thoughts on the development of a rational and modular approach for molecular design in soft matter engineering and proposes ideas of structural and functional synthons for advanced functional materials. It echoes the Materials Genome Initiative by practicing a tentative retro-functional analysis （RFA） scheme. The importance of hierarchical structures in transferring and amplifying molecular functions into macroscopic properties is recognized and emphasized. According to the role of molecular segments in final materials, there are two types of building blocks： structural synthon and functional synthon. Guided by a specific structure for a desired function, these synthons can be modularly combined in various ways to construct molecular scaffolds. Detailed molecular structures are then deduced, designed and synthesized precisely and modularly. While the assembled structure and property may deviate from the original design, the study may allow further refinement of the molecular design toward the target function, The strategy has been used in the development of soft fullerene materials and other giant molecules. There are a few aspects that are not yet well addressed： （1） function and structure are not fully decoupled and （2） the assembled hierarchical structures are sensitive to secondary interactions and molecular geometries across different length scales. Nevertheless, the RFA approach provides a starting point and an alternative thinking pathway by provoking creativity with considerations from both chemistry and physics. This is particularly useful for engineering soft matters with supramolecular lattice formation, as in giant molecules, where the synthons are relatively independent of each other.
