2D Covalent Organic Frameworks with cpt-defect topology Enabled by a Node-Splitting Strategy
Jialiang Liu1, Guangshan Zhou1, Jingming Yang2
1College of Materials Science and Engineering, Zhejiang University of Technology, Hangzhou 310014, China.
Abstract:
Reticular chemistry provides a robust platform for the construction of two-dimensional covalent organic frameworks (2D COFs) with tailored architectures and functionalities. A key synthetic challenge lies in the integration of densely arranged functional moieties without compromising long-range structural order. Herein, we report a node-splitting strategy in which half of the 6-connected C3-symmetric nodes in the cpt topology are replaced by trios of 2-connected C2v-symmetric nodes, generating a new cpt-defect topology. Directional hydrogen bonding among the C2v nodes drives the formation of well-defined hydrogen-bonded nanotraps while preserving crystalline periodicity. The resulting COFs exhibit remarkable performance in gold ion (Au3+) recovery, with COF-36 achieving a maximum adsorption capacity of 1725 mg g-1 and over 99% removal efficiency under strongly acidic conditions. Density functional theory (DFT) calculations attribute this high affinity to the geometric complementarity between the nanotrap cavity and the [AuCl4]- anion, enabling the formation of multiple stabilizing hydrogen bonds. This work establishes node splitting as a versatile approach for topological and functional engineering in COFs, broadening their potential for advanced applications.
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