<br>含有单个钴原子的一维菲基共价有机框架，用于高效的光催化 CO2 还原,Aggregate

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含有单个钴原子的一维菲基共价有机框架，用于高效的光催化 CO2 还原
Aggregate ( IF 13.9 ) Pub Date : 2024-05-08 , DOI: 10.1002/agt2.582
Lv‐Ye Ai ₁ , Qian Wang ₁ , Xiao‐Wen Chen ₂ , Guo‐Fang Jiang ₁

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用于 2D 和 3D 拓扑的金属化共价有机框架（COF）正在不断开发中，而具有 1D 拓扑结构的金属化 COF 仍处于起步阶段。在这里，报道了一种含有 4,4-（1,10-菲咯啉-2,9-二基）双[苯甲醛] （PBA）的新型 1D 菲咯啉基 COF （PAD-COF）。随后，利用 PBA 的双齿配体特性构建金属化的 1D COF，Co SAS/PAD-COF，并通过合成后修饰策略将单个 Co 原子锚定在 PAD-COF 中。该复合物显著提高了 PAD-COF 的光催化性能，优化后的 Co SAS/PAD-COF 的 CO 产率稳定在 3091 μmol ^g-1 ^h-1，选择性为 93%，约为原始 PAD-COF 的 43.7 倍。实验和理论结果表明，由于单个 Co 催化位点和 PAD-COF 的协同作用，Co SAS/PAD-COF具有优异的 CO₂ 光还原活性。其中，PAD-COF 作为宿主，吸附 CO₂ 分子并加载单个 Co 原子。同时，Co 原子起催化位点的作用，促进 CO₂ 的吸附和活化，同时减少 *COOH 中间体形成的反应能垒。因此，这种独特的金属化 1D COF 为光催化还原 CO₂ 提供了一种新的方法。

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

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 PAD-COF. 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.

更新日期：2024-05-08

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