The development of a“two birds with one stone”strategy for capturing pollutant molecules and incorporating new functions provides a promising solution for sustainability.In this work,we designed an unprecedented dee...The development of a“two birds with one stone”strategy for capturing pollutant molecules and incorporating new functions provides a promising solution for sustainability.In this work,we designed an unprecedented deep-cavity aluminum–organic macrocycle to trap dye molecules and enhance non-linear optical performance.Using long building blocks and inorganic aluminum ions at the midriff,we successfully isolated a deep-cavity(1.8 nm)macrocycle,with a deeper cavity than classic pure organic macrocycles,such as crown ether and calixarenes.We report the accurate locking of the HAO7 dye molecule in the deep-cavity macrocycle and reveal its trapping mechanism at the molecular level for the first time.The combined host–vip compound AlOC-136-HAO7 displays altered physical properties,such as a decreased optical band gap and increased proton conductivity but also exhibits enhanced third-order non-linear optical(NLO)properties.Combined with theoretical calculations,we confirmed that the enhancement was attributed to abundant host–vip interactions and the vip-to-vip charge transfer.Our findings provide a strategy for isolating deep-cavity macrocycles and further demonstrate their enormous potential for capturing contaminants and forming valuable materials.展开更多
基金supported by the National Natural Science Foundation of China(22371278,U23A2095,and 92061104)Natural Science Foundation of Fujian Province(2021J06035)Youth Innovation Promotion Association Chinese Academy of Sciences(Y2021081).
文摘The development of a“two birds with one stone”strategy for capturing pollutant molecules and incorporating new functions provides a promising solution for sustainability.In this work,we designed an unprecedented deep-cavity aluminum–organic macrocycle to trap dye molecules and enhance non-linear optical performance.Using long building blocks and inorganic aluminum ions at the midriff,we successfully isolated a deep-cavity(1.8 nm)macrocycle,with a deeper cavity than classic pure organic macrocycles,such as crown ether and calixarenes.We report the accurate locking of the HAO7 dye molecule in the deep-cavity macrocycle and reveal its trapping mechanism at the molecular level for the first time.The combined host–vip compound AlOC-136-HAO7 displays altered physical properties,such as a decreased optical band gap and increased proton conductivity but also exhibits enhanced third-order non-linear optical(NLO)properties.Combined with theoretical calculations,we confirmed that the enhancement was attributed to abundant host–vip interactions and the vip-to-vip charge transfer.Our findings provide a strategy for isolating deep-cavity macrocycles and further demonstrate their enormous potential for capturing contaminants and forming valuable materials.
