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π-Diamond: A Diamondoid Superstructure Driven by π-Interactions
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DOI：10.1002/anie.202409507.png)
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Abstract
En 中文
Modulating the arrangement of superstructures through noncovalent interactions has a significant impact on macroscopic shape and the expression of unique properties. Constructing pi-interaction-driven hierarchical three-dimensional (3D) superstructures poses challenges on account of limited directional control and weak intermolecular interactions. Here we report the construction of a 3D diamondoid superstructure, named pi-Diamond, employing a ditopic strained Z-shaped building block comprising a porphyrin unit as bow-limb double-strapped with two m-xylylene units as bowstrings. This superstructure, reminiscent of diamond's tetrahedral carbon composition, is composed of double-walled tetrahedron (DWT) driven solely by pi-interactions. Hetero-pi-stacking interactions between porphyrin and m-xylylene panels drive the assembly of four building blocks predominantly into a DWT, which undergoes extension to create an adamantane unit and eventually a diamondoid superstructure wherein each porphyrin panel is shared by two neighboring tetrahedra through hetero-pi-stacking. pi-Diamond exhibits a solid-state fluorescent quantum yield 44 times higher than that of tetraphenylporphyrin along with excellent photocatalytic performance. The precise 3D directionality of pi-interactions, achieved through strained multipanel building blocks, revolutionizes the assembly of hierarchical 3D superstructures driven by pi-interactions. We created a 3D diamondoid superstructure called pi-Diamond using a strained Z-shaped building block with a porphyrin unit and two m-xylylene units. It resembles diamond's structure and is driven purely by pi-interactions. Hetero-pi-stacking assembles four building blocks into an extendable double-walled tetrahedron, forming an adamantane unit and the diamondoid superstructure. image
Keywords:
Noncovalent Interactions
Self-Assembly
Crystal Engineering
Diamondoid Superstructure
Porphyrin
Journal
IF:
16.9
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5.7W
Citations:
53.0W