Unveiling the mechanism of enhanced water purification by F-Fe-Zn-MCM-41 in O3/PMS

IF 20.2 1区化学 Q1 CHEMISTRY, PHYSICAL

Applied Catalysis B: Environmental Pub Date : 2024-01-02 DOI:10.1016/j.apcatb.2023.123608

Weirui Chen , Yingjing Tian , Dongpo Liu , Yunqiang Yi , Xukai Li , Jing Wang , Liying Bin , Ping Li , Bing Tang , Laisheng Li

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Abstract

To break the restriction of SO₅^2- as the essential initiator in O₃/PMS reaction during water purification, F-Fe-Zn-MCM-41 (FFeZn-M) was designed to enhance ibuprofen (IBP) degradation during O₃/PMS process. The great electronegativity difference between Fe and Zn created an electron flow from Zn to Fe, which was further enhanced by electron withdrawing Si-F group. FFeZn-M changed the traditional interaction between PMS and O₃. PMS would be adsorbed on the surface of Zn and acted as an electron donor. Meanwhile, O₃ received electrons from Fe site and was activated into ROS. With •OH and ¹O₂ as the main ROS, FFeZn-M/O₃/PMS process achieved the complete IBP removal and a 60.9% mineralization rate, which was significantly higher over those of FFeZn-M/O₃ and FFeZn-M/PMS processes. FFeZn-M/O₃/PMS behaved better at weak acidic and neutral condition rather than the basic condition required by conventional O₃/PMS process. This study offered a novel catalyst design strategy for O₃/PMS.

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揭示 F-Fe-Zn-MCM-41 在 O3/PMS 中增强水净化的机理

为了打破 SO52- 作为水净化过程中 O3/PMS 反应的基本引发剂的限制，我们设计了 F-Fe-Zn-MCM-41（FFeZn-M）来增强 O3/PMS 过程中布洛芬（IBP）的降解。铁和锌之间巨大的电负性差异产生了从锌到铁的电子流，而电子撤回的 Si-F 基团进一步增强了这种电子流。FFeZn-M 改变了 PMS 和 O3 之间传统的相互作用。PMS 会吸附在 Zn 表面，并充当电子供体。同时，O3 从 Fe 位点获得电子，并被活化成 ROS。以 -OH 和 1O2 为主要 ROS，FFeZn-M/O3/PMS 工艺实现了对 IBP 的完全去除，矿化率达到 60.9%，明显高于 FFeZn-M/O3 和 FFeZn-M/PMS 工艺。FFeZn-M/O3/PMS 在弱酸性和中性条件下的表现比传统 O3/PMS 工艺要求的碱性条件更好。这项研究为 O3/PMS 工艺提供了一种新型催化剂设计策略。

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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.