Dynamic Stereochemistry of M8Pd6 Supramolecular Cages Based on Metal‐Center Lability for Differential Chiral Induction, Resolution, and Recognition

Author:

Huang Yin‐Hui1,Lu Yu‐Lin1,Zhang Xiao‐Dong1,Liu Chen‐Hui1,Ruan Jia1,Qin Yu‐Han1,Cao Zhong‐Min1,Jiang Jijun1,Xu Hai‐Sen1,Su Cheng‐Yong1ORCID

Affiliation:

1. MOE Laboratory of Bioinorganic and Synthetic Chemistry GBRCE for Functional Molecular Engineering LIFM, IGCME School of Chemistry Sun Yat-Sen University Guangzhou 510275 China

Abstract

AbstractA series of isostructural supramolecular cages with a rhombic dodecahedron shape have been assembled with distinct metal‐coordination lability (M8Pd6‐MOC‐16, M=Ru2+, Fe2+, Ni2+, Zn2+). The chirality transfer between metal centers generally imposes homochirality on individual cages to enable solvent‐dependent spontaneous resolution of Δ8/Λ8−M8Pd6 enantiomers; however, their distinguishable stereochemical dynamics manifests differential chiral phenomena governed by the cage stability following the order Ru8Pd6>Ni8Pd6>Fe8Pd6>Zn8Pd6. The highly labile Zn centers endow the Zn8Pd6 cage with conformational flexibility and deformation, enabling intrigue chiral‐Δ8/Λ8−Zn8Pd6 to meso‐Δ4Λ4−Zn8Pd6 transition induced by anions. The cage stabilization effect differs from inert Ru2+, metastable Fe2+/Ni2+, and labile Zn2+, resulting in different chiral‐guest induction. Strikingly, solvent‐mediated host–guest interactions have been revealed for Δ8/Λ8−(Ru/Ni/Fe)8Pd6 cages to discriminate the chiral recognition of the guests with opposite chirality. These results demonstrate a versatile procedure to control the stereochemistry of metal‐organic cages based on the dynamic metal centers, thus providing guidance to maneuver cage chirality at a supramolecular level by virtue of the solvent, anion, and guest to benefit practical applications.

Funder

Ministry of Science and Technology of the People's Republic of China

National Natural Science Foundation of China

Guangdong Provincial Department of Science and Technology

China Postdoctoral Science Foundation

Publisher

Wiley

Subject

General Chemistry,Catalysis

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