Peroxymonosulfate enhanced photocatalytic degradation of serial bisphenols by metal-free covalent organic frameworks under visible light irradiation: mechanisms, degradation pathway and DFT calculation

IF 13.3 1区 工程技术 Q1 ENGINEERING, CHEMICAL Chemical Engineering Journal Pub Date : 2022-02-15 DOI:10.1016/j.cej.2021.132833
Fuyang Liu, Qiqi Dong, Chenyi Nie, Zhengmao Li, Boaiqi Zhang, Peng Han, Wulin Yang, Meiping Tong
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引用次数: 28

Abstract

Visible light driven peroxymonosulfate (PMS) activation by metal-free photocatalysts has attracted great attention. In present study, covalent organic frameworks (COF-PRD, PRD refers to pyridine) were synthesized and utilized to activate PMS to degrade bisphenol A (BPA) with visible light (VL) irradiation. COF-PRD with PMS improved 3.5 times degradation kinetics for BPA degradation relative to that of COF-PRD without PMS with VL irradiation. ·O2, h+ and 1O2 dominated the BPA degradation in COF-PRD with PMS with VL irradiation. Under anaerobic condition, BPA could still be effectively degraded due to the reaction of PMS with e to generate ·SO4. In addition to BPA, bisphenol F (BPF), bisphenol B (BPB), bisphenol Z (BPZ) and bisphenol AP (BPAP) could also be effectively degraded by COF-PRD with PMS under VL irradiation conditions. Density functional theory (DFT) calculation together with intermediates determination showed that the main degradation pathway of bisphenols (BPs) included hydroxylation, electrophilic attack and ring-opening reaction. The bioaccumulation effects of BPs were greatly reduced during the degradation process. Moreover, COF-PRD exhibited excellent reusability in ten successive cycles. Clearly, COF-PRD could be employed as photocatalytic PMS activation to degrade bisphenols under both aerobic and anaerobic conditions.

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过氧单硫酸盐增强可见光下无金属共价有机骨架光催化降解双酚类化合物的机理、降解途径及DFT计算
无金属光催化剂在可见光下活化过氧单硫酸盐(PMS)引起了广泛的关注。本研究合成了共价有机骨架(COF-PRD, PRD指吡啶),并利用可见光(VL)照射激活PMS降解双酚A (BPA)。添加PMS的COF-PRD在VL照射下对BPA的降解动力学比不添加PMS的COF-PRD提高了3.5倍。·VL辐照下PMS对COF-PRD中BPA的降解主要是O2 -、h+和1O2。在厌氧条件下,PMS与e -反应生成·SO4 -,仍能有效降解BPA。除双酚a外,双酚F (BPF)、双酚B (BPB)、双酚Z (BPZ)和双酚AP (BPAP)在VL辐照条件下也能被COF-PRD与PMS有效降解。密度泛函理论(DFT)计算和中间体测定表明,双酚类化合物的主要降解途径包括羟基化、亲电攻击和开环反应。在降解过程中,bp的生物积累效应大大降低。此外,COF-PRD在10个连续循环中表现出良好的可重复使用性。显然,COF-PRD可以作为光催化PMS活化在好氧和厌氧条件下降解双酚。
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来源期刊
Chemical Engineering Journal
Chemical Engineering Journal 工程技术-工程:化工
CiteScore
21.70
自引率
9.30%
发文量
6781
审稿时长
2.4 months
期刊介绍: The Chemical Engineering Journal is an international research journal that invites contributions of original and novel fundamental research. It aims to provide an international platform for presenting original fundamental research, interpretative reviews, and discussions on new developments in chemical engineering. The journal welcomes papers that describe novel theory and its practical application, as well as those that demonstrate the transfer of techniques from other disciplines. It also welcomes reports on carefully conducted experimental work that is soundly interpreted. The main focus of the journal is on original and rigorous research results that have broad significance. The Catalysis section within the Chemical Engineering Journal focuses specifically on Experimental and Theoretical studies in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. These studies have industrial impact on various sectors such as chemicals, energy, materials, foods, healthcare, and environmental protection.
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