Issue 16, 2024

Dynamic covalent bonding for directed construction of molecular cages toward carbon dioxide reduction

Abstract

Zirconium-based metal–organic cages (Zr-MOCs) have garnered attention for their notable stability and enduring porosity. However, the rational design and precise synthesis of these structures remain challenging. In this context, we introduce a method that utilizes a dynamic covalent bond construction strategy for the meticulous stepwise synthesis of metal–organic cages. By applying this approach, a novel lantern-like metal–organic cage is synthesized (Schiff-base ZrOC-1). The Schiff-base ZrOC-1 was then investigated for photocatalytic carbon dioxide (CO2) reduction. Notably, unlike the negligible catalytic activity of the precursor (Zr-CHO) and Zr-MOC without dynamic covalent bonds (ZrT-1), Schiff-base ZrOC-1 exhibits outstanding catalytic performance, converting CO2 into CO with a yield of 2.55 mmol g−1 h−1. Experimental evidence suggests that the dynamic covalent bonds present within Schiff-base ZrOC-1 serve as the active sites for photocatalytic CO2 reduction, and the cage's structure itself contributes positively to the photocatalytic activity.

Graphical abstract: Dynamic covalent bonding for directed construction of molecular cages toward carbon dioxide reduction

Supplementary files

Article information

Article type
Research Article
Submitted
25 Apr 2024
Accepted
18 Jun 2024
First published
20 Jun 2024

Inorg. Chem. Front., 2024,11, 5120-5126

Dynamic covalent bonding for directed construction of molecular cages toward carbon dioxide reduction

J. He, M. Dong, Y. Zhao, D. Cui, X. Yao, F. Meng, W. Li, S. Yang, C. Sun and Z. Su, Inorg. Chem. Front., 2024, 11, 5120 DOI: 10.1039/D4QI01043D

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