Zwitterionic and Hydrophilic Vinylene-Linked Covalent Organic Frameworks for Efficient Photocatalytic Hydrogen Evolution,ACS Applied Materials & Interfaces

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Zwitterionic and Hydrophilic Vinylene-Linked Covalent Organic Frameworks for Efficient Photocatalytic Hydrogen Evolution
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2023-07-25 , DOI: 10.1021/acsami.3c08250
Haifeng Ji ₁ , Danyang Qiao ₂ , Gaojie Yan ₁ , Beibei Dong ₂ , Yi Feng ₁ , Xiongwei Qu ₁ , Yu Jiang ₃ , Xiaojie Zhang ₁

Affiliation

Developing effective synthetic strategies as well as broadening functionalities for zwitterionic materials that comprise moieties with equimolar cationic and anionic groups still remains a huge challenge. Herein, we develop two zwitterionic vinylene-linked covalent organic frameworks (Zi-VCOF-1 and Zi-VCOF-2) that are a type of novel hydrophilic material. Zi-VCOF-1 and Zi-VCOF-2 are obtained directly through the convenient Knoevenagel condensation of new sulfonic-pyridinium zwitterionic monomers with aromatic aldehyde derivatives. This is the first report on zwitterionic COFs being constructed by the bottom-up functionalization approach from predesigned zwitterionic monomers. Both Zi-VCOFs exhibit a high photocatalytic hydrogen evolution rate (HER) because of their appropriate optical property and outstanding hydrophilicity. Specifically, Zi-VCOF-1 and Zi-VCOF-2 show photocatalytic HER of 13,547 and 5057 μmol h^–1 g^–1, respectively. Interestingly, the photocatalytic HER of Zi-VCOF-1 is about 2.68 times of that of Zi-VCOF-2, although they differ by only one methyl group in sulfonic-pyridinium zwitterionic pairs. The photocatalytic HER of Zi-VCOF-1 is not only the highest in the vinylene-linked COFs but also outstanding among the most reported COFs. This is the first application of zwitterionic COFs for photocatalytic hydrogen evolution, which would open a new frontier in zwitterionic COFs and be helpful for the design of other photocatalytic materials.

中文翻译：

用于高效光催化析氢的两性离子和亲水性亚乙烯基连接的共价有机框架

开发有效的合成策略以及拓宽包含等摩尔阳离子和阴离子基团的两性离子材料的功能仍然是一个巨大的挑战。在此，我们开发了两种两性离子亚乙烯基连接的共价有机骨架（Zi-VCOF-1和Zi-VCOF-2），它们是一种新型亲水材料。Zi-VCOF-1 和 Zi-VCOF-2 是通过新型磺基吡啶鎓两性离子单体与芳香醛衍生物进行方便的 Knoevenagel 缩合直接获得的。这是关于通过自下而上的功能化方法从预先设计的两性离子单体构建两性离子COF的第一份报告。这两种 Zi-VCOF 由于其适当的光学性质和出色的亲水性而表现出高光催化析氢速率（HER）。具体而言，Zi-VCOF-1 和 Zi-VCOF-2 的光催化 HER 值分别为 13,547 和 5057 μmol h ^–1 g ^{–1 。}有趣的是，Zi-VCOF-1 的光催化 HER 约为 Zi-VCOF-2 的 2.68 倍，尽管它们在磺酸吡啶鎓两性离子对中仅存在一个甲基不同。Zi-VCOF-1 的光催化 HER 不仅是亚乙烯基连接的 COF 中最高的，而且在报道最多的 COF 中也很突出。这是两性离子COF在光催化析氢方面的首次应用，这将开辟两性离子COF的新领域，并有助于其他光催化材料的设计。

更新日期：2023-07-25

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