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Clickable Norbornene-Based Zirconium Carboxylate Polyhedra
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DOI：10.1021/acs.chemmater.2c03252.png)
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Abstract
En 中文
A common way to modify the properties of metal- organic polyhedra (MOPs) is to install pendant functionalities on the organic bridging ligands. These groups can then participate in coupling reactions to further decorate a given architecture. Via exploitation of click chemistry, it is possible to access a diverse library of MOPs that share a common core, which can reduce both synthetic complexity and cost. Herein, we report the formation of a reactive norbornene-based MOP through a one-pot tandem coordination-driven self-assembly/Diels-Alder reaction between fumaric acid and zirconocene dichloride (Cp2ZrCl2). The generality of this tandem process was illustrated by the subsequent synthesis of a norbornene-based Zr cluster formed from maleic acid and Cp2ZrCl2. We demonstrate post-assembly modification of this cage using versatile thiol-ene click chemistry, resulting in the formation of either individual functionalized MOPs or cross-linked polymer/MOP hybrid composites. The physical properties of these composites can be controlled by the addition of poly(ethylene glycol) diacrylate as a co-monomer, allowing for the synthesis of free-standing, flexible films at MOP loadings of 30-60% (w/w). These results demonstrate the effectiveness of thiol-ene click chemistry as a method of MOP functionalization, expanding the toolbox for the synthesis of new advanced materials.
Keywords:
METAL-ORGANIC POLYHEDRA
THIOL-ENE
COORDINATION CAGES
DESIGN
FUNCTIONALIZATION
HYDROCARBONS
FRAMEWORKS
CHEMISTRY
MEMBRANES
NANOCAGES
Journal
IF:
7
Papers:
2.8W
Citations:
11.4W