Integrating Suitable Linkage of Covalent Organic Frameworks into Covalently Bridged Inorganic/Organic Hybrids toward Efficient Photocatalysis,Journal of the American Chemical Society

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Integrating Suitable Linkage of Covalent Organic Frameworks into Covalently Bridged Inorganic/Organic Hybrids toward Efficient Photocatalysis
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2020-02-19 , DOI: 10.1021/jacs.0c00054
Hou Wang ₁ , Cheng Qian ₁ , Jia Liu ₂ , Yongfei Zeng ₃ , Dongdong Wang ₁ , Weiqiang Zhou ₁ , Long Gu ₁ , Hongwei Wu ₁ , Guofeng Liu ₁ , Yanli Zhao ₁

Affiliation

Covalent organic frameworks (COFs) are excellent platforms with tailored functionalities in photocatalysis. There are still challenges in increasing photochemical performance of COFs. Therefore, we designed and prepared a series of COFs for photocatalytic hydrogen generation. Varying different ratios of β-ketoenamine to imine moieties in the linkages could differ the ordered structure, visible light harvesting and bandgap. Overall β-ketoenamine linked-COFs exhibited much better photocatalytic activity than those COFs having both β-ketoenamine and imine moieties on account of non-quenched excited-state and more favorable HOMO level in photoinduced oxidation reaction from the former. Specifically, after in situ growth of β-ketoenamine linked COFs onto NH2-Ti3C2Tx (Tx = -O and -OH) MXene via covalent connection, the hetero-hybrid showed an obvious improvement in photocatalytic H2 evolution because of strong covalent coupling, electrical conductivity and efficient charge transfer. This integrated linkage evolution and covalent hybridization approach advances the development of COF-based photocatalysts.

中文翻译：

将共价有机骨架的合适连接整合到共价桥接的无机/有机杂化物中以实现高效的光催化

共价有机框架 (COF) 是在光催化中具有定制功能的优秀平台。在提高 COF 的光化学性能方面仍然存在挑战。因此，我们设计并制备了一系列用于光催化制氢的COFs。改变连接中 β-酮烯胺与亚胺部分的不同比例可能会导致有序结构、可见光捕获和带隙不同。总体而言，β-酮烯胺连接的 COFs 表现出比同时具有 β-酮烯胺和亚胺部分的那些 COFs 更好的光催化活性，这是由于非猝灭的激发态和更有利的 HOMO 能级在光诱导氧化反应中来自前者。具体而言，在 β-酮烯胺连接的 COFs 通过共价连接原位生长到 NH2-Ti3C2Tx（Tx = -O 和 -OH）MXene 上之后，由于强共价耦合、导电性和有效的电荷转移，异源杂化物在光催化析氢方面表现出明显的改善。这种集成的连接进化和共价杂交方法促进了基于 COF 的光催化剂的开发。

更新日期：2020-02-19

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