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通过一锅多组分反应在共价有机框架中整合双功能和化学稳定性用于太阳能驱动的过氧化氢生产

Integrating Bifunctionality and Chemical Stability in Covalent Organic Frameworks via One-Pot Multicomponent Reactions for Solar-Driven HO Production.

作者信息

Das Prasenjit, Chakraborty Gouri, Roeser Jérôme, Vogl Sarah, Rabeah Jabor, Thomas Arne

机构信息

Department of Chemistry/Functional Materials, Technische Universität Berlin, 10623 Berlin, Germany.

BAM Federal Institute for Materials Research and Testing, Richard-Willstätter-Str. 11, 12489 Berlin, Germany.

出版信息

J Am Chem Soc. 2023 Feb 8;145(5):2975-2984. doi: 10.1021/jacs.2c11454. Epub 2023 Jan 25.

Abstract

Multicomponent reactions (MCRs) can be used to introduce different functionalities into highly stable covalent organic frameworks (COFs). In this work, the irreversible three-component Doebner reaction is utilized to synthesize four chemically stable quinoline-4-carboxylic acid DMCR-COFs ( and ) equipped with an acid-base bifunctionality. These DMCR-COFs show superior photocatalytic HO evolution (one of the most important industrial oxidants) compared to the imine COF analogue (). This is achieved with sacrificial oxidants but also in pure water and under an oxygen or air atmosphere. Furthermore, the DMCR-COFs show high photostability, durability, and recyclability. MCR-COFs thus provide a viable materials' platform for solar to chemical energy conversion.

摘要

多组分反应(MCRs)可用于将不同功能基团引入高度稳定的共价有机框架(COFs)中。在这项工作中,利用不可逆的三组分Doebner反应合成了四种具有酸碱双功能的化学稳定的喹啉-4-羧酸DMCR-COFs( 和 )。与亚胺COF类似物( )相比,这些DMCR-COFs表现出优异的光催化析氢性能(最重要的工业氧化剂之一)。这不仅在使用牺牲性氧化剂的情况下实现,而且在纯水以及氧气或空气气氛下也能实现。此外,DMCR-COFs还表现出高光稳定性、耐久性和可回收性。因此,MCR-COFs为太阳能到化学能的转化提供了一个可行的材料平台。

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