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可见光下浮动氧空位-CuFeO光催化剂活化过一硫酸盐用于高效降解磺胺二甲嘧啶

Activation of peroxymonosulfate by a floating oxygen vacancies - CuFeO photocatalyst under visible light for efficient degradation of sulfamethazine.

作者信息

Sun Qiunan, Wang Xuejiang, Liu Yiyang, Xia Siqing, Zhao Jianfu

机构信息

State Key Laboratory of Pollution Control and Resource Reuse, College of Environmental Science and Engineering, Tongji University, Shanghai 200092, PR China; Shanghai Institute of Pollution Control and Ecological Security, Shanghai 200092, PR China.

State Key Laboratory of Pollution Control and Resource Reuse, College of Environmental Science and Engineering, Tongji University, Shanghai 200092, PR China.

出版信息

Sci Total Environ. 2022 Jun 10;824:153630. doi: 10.1016/j.scitotenv.2022.153630. Epub 2022 Feb 14.

Abstract

In this study, expanded perlite supported oxygen vacancies-CuFeO (OVs-CFEp) was synthesized via a simple method and utilized as floating catalyst to activate peroxymonosulfate (PMS) for the removal of sulfamethazine (SMT) under visible light irradiation. OVs-CFEp/Vis/PMS synergy presents much superior performance than that of OVs-CFEp/Vis system and OVs-CFEp/PMS system. PMS was efficiently activated by OVs-CFEp at a wide range of pH values, while the degrading rate of SMT was up to 95% in OVs-CFEp/Vis/PMS system. Oxygen vacancies and ·O accelerated the conversion of Fe(III)/Fe(II) and Cu(I)/Cu(II). The combination of the floating loader boosted light absorption capacity and sufficiently prevented metal ions leaching, which was all beneficial to enhance catalytic performance and recyclability. Besides, the reactive oxygen species were investigated systematically, proving that visible light and OVs-CFEp could activate PMS to produce ·SO, ·OH, O·, and O reactive species. Furthermore, based on intermediates identification and Density Functional Theory (DFT) calculation, three types and seven main degradation pathways involving cleavage of bond, SMT molecular rearrangement, and hydroxylation reaction were proposed. So this high photo-absorbing catalyst coupling with advanced oxidation progress was promising for extensive environmental remediation.

摘要

在本研究中,通过一种简单的方法合成了膨胀珍珠岩负载的氧空位 - 铜铁氧化物(OVs-CFEp),并将其用作浮动催化剂,在可见光照射下活化过一硫酸盐(PMS)以去除磺胺二甲嘧啶(SMT)。OVs-CFEp/可见光/PMS协同作用表现出比OVs-CFEp/可见光体系和OVs-CFEp/PMS体系更优异的性能。OVs-CFEp在较宽的pH值范围内有效活化PMS,而在OVs-CFEp/可见光/PMS体系中SMT的降解率高达95%。氧空位和·O加速了Fe(III)/Fe(II)和Cu(I)/Cu(II)的转化。浮动载体的结合提高了光吸收能力并充分防止了金属离子浸出,这都有利于提高催化性能和可回收性。此外,对活性氧物种进行了系统研究,证明可见光和OVs-CFEp可以活化PMS产生·SO、·OH、O·和O活性物种。此外,基于中间体鉴定和密度泛函理论(DFT)计算,提出了三种类型和七条主要降解途径,包括键断裂、SMT分子重排和羟基化反应。因此,这种高光吸收催化剂与高级氧化过程相结合在广泛的环境修复方面具有前景。

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