Constructing bifunctional and robust covalent organic frameworks via three-component one-pot Doebner reaction for Cr(VI) removal

IF 20.2 1区化学 Q1 CHEMISTRY, PHYSICAL

Applied Catalysis B: Environmental Pub Date : 2023-12-29 DOI:10.1016/j.apcatb.2023.123672

Muzammil Hussain , Anam Saddique , Kamakshaiah Charyulu Devarayapalli , Bolam Kim , In Woo Cheong , Dae Sung Lee

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Abstract

The integral part of covalent organic frameworks (COFs) is covalent bonds. Thus, stable and functional links must be developed to expand the potential applications of COFs. Herein, in situ linkage functionalization using a three-component irreversible Doebner reaction was achieved to fabricate chemically stable carboxylic acid-bearing COFs (Tp-Tta-COOH and Tp-Tapb-COOH), which have abundant chelating groups and ordered electron donor–acceptor moieties facilitating charge separation for effective Cr(VI) adsorption and photoreduction, respectively. These functionalized COFs are more effective at Cr(VI) removal via adsorption and photoreduction than their unfunctionalized counterparts (Tp-Tta and Tp-Tapb). The synergy of adsorption and photocatalysis is crucial to effectively remove Cr(VI) from aqueous solutions. This synergy empowers Tp-Tta-COOH to be used continuously for Cr(VI) removal without any elution after each cycle. Furthermore, Tp-Tta-COOH exhibits high chemical stability, durability, and recyclability. This study will promote the development of durable and useful COF materials for real-world applications.

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通过三组分单锅多布纳反应构建双功能强韧共价有机框架以去除六价铬

共价有机框架（COFs）的组成部分是共价键。因此，必须开发稳定的功能性连接，以拓展 COF 的潜在应用。本文利用三组份不可逆多布纳反应实现了原位连接功能化，制备出化学性质稳定的含羧酸的 COF（Tp-Tta-COOH 和 Tp-Tapb-COOH），它们具有丰富的螯合基团和有序的电子供体-受体分子，可促进电荷分离，从而分别实现对六价铬的有效吸附和光氧化还原。与未官能化的同类产品（Tp-Tta 和 Tp-Tapb）相比，这些官能化 COF 通过吸附和光诱导去除六价铬的效果更好。吸附和光催化的协同作用对于从水溶液中有效去除六价铬至关重要。这种协同作用使 Tp-Tta-COOH 能够连续用于去除六价铬，而无需在每次循环后进行洗脱。此外，Tp-Tta-COOH 还具有很高的化学稳定性、耐久性和可回收性。这项研究将促进为实际应用开发耐用、有用的 COF 材料。

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来源期刊

Applied Catalysis B: Environmental 环境科学-工程：化工

CiteScore

38.60

自引率

6.30%

发文量

1117

审稿时长

24 days

期刊介绍： Applied Catalysis B: Environment and Energy (formerly Applied Catalysis B: Environmental) is a journal that focuses on the transition towards cleaner and more sustainable energy sources. The journal's publications cover a wide range of topics, including: 1.Catalytic elimination of environmental pollutants such as nitrogen oxides, carbon monoxide, sulfur compounds, chlorinated and other organic compounds, and soot emitted from stationary or mobile sources. 2.Basic understanding of catalysts used in environmental pollution abatement, particularly in industrial processes. 3.All aspects of preparation, characterization, activation, deactivation, and regeneration of novel and commercially applicable environmental catalysts. 4.New catalytic routes and processes for the production of clean energy, such as hydrogen generation via catalytic fuel processing, and new catalysts and electrocatalysts for fuel cells. 5.Catalytic reactions that convert wastes into useful products. 6.Clean manufacturing techniques that replace toxic chemicals with environmentally friendly catalysts. 7.Scientific aspects of photocatalytic processes and a basic understanding of photocatalysts as applied to environmental problems. 8.New catalytic combustion technologies and catalysts. 9.New catalytic non-enzymatic transformations of biomass components. The journal is abstracted and indexed in API Abstracts, Research Alert, Chemical Abstracts, Web of Science, Theoretical Chemical Engineering Abstracts, Engineering, Technology & Applied Sciences, and others.