Subject Code:B01With the financial support from the National Natural Science Foundation of China,the research group led by Prof.Sun Qingfu(孙庆福)from the Fujian Institute of Research on the Structure of Matter,Chines...Subject Code:B01With the financial support from the National Natural Science Foundation of China,the research group led by Prof.Sun Qingfu(孙庆福)from the Fujian Institute of Research on the Structure of Matter,Chinese Academy of Sciences has recently reported a dynamic anion-adaptive self-assembly system展开更多
In nature,enzymes at specific folded conformations exhibit high substrate complementarity,enabling them to efficiently and selectively catalyze biochemical reactions.Inspired by enzymes,coordination cages with conform...In nature,enzymes at specific folded conformations exhibit high substrate complementarity,enabling them to efficiently and selectively catalyze biochemical reactions.Inspired by enzymes,coordination cages with conformational dynamics have been designed and are receiving increasing attention due to their versatile applications in allosteric guest binding and catalysis.We present here two enzyme-mimicking adaptive macrocycle-based coordination cages,Pd_(2)L_(2)^(1) and Pd_(2)L_(2)^(2),from macrocycle-based ligands(L^(1) and L^(2))and the encapsulation and stabilization of Lindqvist polyoxometalates anions M6O192−(M=W or Mo)in neutral aqueous solution.X-ray crystallographic studies have verified the formation of 1:1 host-guest complexes of two Pd_(2)L_(2) cages and the W6O192−anion,via an induced-fit folding mechanism.Compared with the free host,Pd_(2)L_(2)^(1) exhibited an induced-fit semi-folded conformation in the inclusion complex,while Pd_(2)L_(2)^(2) adopted an induced-fit fully-folded conformation.Moreover,the Mo_(6)O_(19)⊂Pd_(2)L_(2) host-guest complexes demonstrate high yield and selectivity in the oxidative decontamination reaction of the sulfur mustard simulant,2-chloroethyl ethyl sulfide.This work not only sheds light on the importance of conformational adaptability in enzyme-like systems but also paves the way for protecting labile POM clusters via host-guest encapsulation toward enhanced catalytic performance in aqueous solution.展开更多
文摘Subject Code:B01With the financial support from the National Natural Science Foundation of China,the research group led by Prof.Sun Qingfu(孙庆福)from the Fujian Institute of Research on the Structure of Matter,Chinese Academy of Sciences has recently reported a dynamic anion-adaptive self-assembly system
基金supported by the National Key Research and Development Program of China(2022YFA1503300,2021YFA1500400)the National Natural Science Foundation of China(22171262,22171264,22201285)the Science Foundation of Fujian Province(2021J01516,2021J02016).
文摘In nature,enzymes at specific folded conformations exhibit high substrate complementarity,enabling them to efficiently and selectively catalyze biochemical reactions.Inspired by enzymes,coordination cages with conformational dynamics have been designed and are receiving increasing attention due to their versatile applications in allosteric guest binding and catalysis.We present here two enzyme-mimicking adaptive macrocycle-based coordination cages,Pd_(2)L_(2)^(1) and Pd_(2)L_(2)^(2),from macrocycle-based ligands(L^(1) and L^(2))and the encapsulation and stabilization of Lindqvist polyoxometalates anions M6O192−(M=W or Mo)in neutral aqueous solution.X-ray crystallographic studies have verified the formation of 1:1 host-guest complexes of two Pd_(2)L_(2) cages and the W6O192−anion,via an induced-fit folding mechanism.Compared with the free host,Pd_(2)L_(2)^(1) exhibited an induced-fit semi-folded conformation in the inclusion complex,while Pd_(2)L_(2)^(2) adopted an induced-fit fully-folded conformation.Moreover,the Mo_(6)O_(19)⊂Pd_(2)L_(2) host-guest complexes demonstrate high yield and selectivity in the oxidative decontamination reaction of the sulfur mustard simulant,2-chloroethyl ethyl sulfide.This work not only sheds light on the importance of conformational adaptability in enzyme-like systems but also paves the way for protecting labile POM clusters via host-guest encapsulation toward enhanced catalytic performance in aqueous solution.
