One-dimensional phenanthroline-based covalent organic framework bearing single cobalt atoms for efficient photocatalytic CO₂ reduction

Abstract

Metalated covalent organic frameworks (COFs) for 2D and 3D topologies are continuously being developed, whereas metalated COFs with 1D topologies are still in their infancy. Here, a novel 1D phenanthroline-based COF containing 4,4- (1,10-phenanthroline-2,9-diyl)bis[benzaldehyde] (PBA) is reported (PAD-COF). Subsequently, a metalated 1D COF, Co SAS/PAD-COF, is constructed using the bidentate ligand properties of PBA and anchoring the single Co atoms in PAD-COF through a post-synthetic modification strategy. This complex significantly improved the photocatalytic performance of PAD-COF, and the CO yield of the optimized Co SAS/PAD-COF was stable at 3091 μmol g⁻¹ h⁻¹ with a selectivity of 93%, which is approximately 43.7 times that of the original PAD-COF. Experimental and theoretical results demonstrate the excellent CO₂ photoreduction activity of Co SAS/PAD-COF owing to the synergistic effect of single Co catalytic sites and PADCOF. Among them, PAD-COF, as the host, adsorbs CO₂ molecules and loads single Co atoms. Meanwhile, Co atoms function as catalytic sites and promote the adsorption and activation of CO₂, while reducing the reaction energy barrier formed by the *COOH intermediates. Therefore, this unique metalated 1D COF provides a fresh approach to photocatalytic CO₂ reduction.

Keywords

1D phenanthroline-based covalent organic framework / metalated / photocatalytic CO ₂ reduction / single Co atoms

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RIGHTS & PERMISSIONS

2024 The Author(s). Aggregate published by SCUT, AIEI, and John Wiley & Sons Australia, Ltd.