Novel oxidant-free VUV/Fe2+/oxalate process for high-efficiency removal of norfloxacin: Oxidation performance and synergistic mechanism

IF 13.3 1区工程技术 Q1 ENGINEERING, CHEMICAL

Chemical Engineering Journal Pub Date : 2024-11-19 DOI:10.1016/j.cej.2024.157779

Chuang Wang, Xiaohui Wang, Jinying Du, Renjian Deng, Bozhi Ren, Wenhao Wang, Baolin Hou, Bingzhi Liu, Zhiwei Zhao

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Abstract

Based on Vacuum UV (VUV) in situ cracking water to generate reactive oxygen species (ROS) and promote Fe²⁺/Fe³⁺ redox cycle, a novel oxidant-free VUV/Fe²⁺/oxalate (Ox) homogeneous oxidation process was built to efficiently degrade norfloxacin (NOR). The performance and synergistic mechanism of VUV/Fe²⁺/Ox for NOR degradation under near-neutral conditions were investigated. Compared with sub-processes, VUV/Fe²⁺/Ox obviously accelerated NOR oxidation and reduced energy consumption, and its synergistic factor of NOR removal was 2.32. Effects of operating parameters Fe²⁺, Ox dose and solution pH on VUV/Fe²⁺/Ox and their mechanisms were analyzed. Synergistic mechanisms of NOR degradation via VUV/Fe²⁺/Ox, such as in situ generation of H₂O₂, Fe²⁺/Fe³⁺ redox cycle, ROS characterization and contribution analysis, NOR degradation pathways and its toxicity changes were also investigated. Through the use of ROS fluorescence characterizations and quenching experiments, hydroxyl radical and superoxide radical were identified as primary ROS in VUV/Fe²⁺/Ox, and their contributions to NOR degradation were 73.17 % and 20.91 %, respectively. Besides, synergistic mechanisms of VUV/Fe²⁺/Ox process, which mainly included the respective roles of VUV irradiation, Fe²⁺ and Ox, were also recommended. Furthermore, effects of chelators and water matrices on NOR degradation via VUV/Fe²⁺/Ox were also researched. VUV/Fe²⁺/Ox process showed satisfactory NOR degradation effects in actual waters, indicating its practical application potential. The degradation of NOR by novel VUV/Fe²⁺/Ox process significantly reduced its environmental and health hazards.

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高效去除诺氟沙星的新型无氧化剂紫外/Fe2+/草酸盐工艺：氧化性能和协同机制

基于真空紫外（VUV）原位裂解水产生活性氧（ROS）并促进 Fe2+/Fe3+ 氧化还原循环的原理，建立了一种新型的无氧化剂 VUV/Fe2+/草酸盐（Ox）均相氧化工艺，用于高效降解诺氟沙星（NOR）。研究了紫外/Fe2+/Ox 在近中性条件下降解 NOR 的性能和协同机制。与其他子过程相比，紫外/Fe2+/Ox明显加速了NOR的氧化，降低了能耗，其去除NOR的协同系数为2.32。分析了操作参数 Fe2+、Ox 剂量和溶液 pH 对紫外/Fe2+/Ox 的影响及其机理。此外，还研究了紫外/Fe2+/Ox 降解 NOR 的协同机制，如原位生成 H2O2、Fe2+/Fe3+ 氧化还原循环、ROS 特征和贡献分析、NOR 降解途径及其毒性变化。通过 ROS 荧光表征和淬灭实验，确定羟自由基和超氧自由基是紫外/Fe2+/Ox 中的主要 ROS，它们对 NOR 降解的贡献率分别为 73.17 % 和 20.91 %。此外，还提出了紫外/Fe2+/Ox 过程的协同机制，主要包括紫外辐照、Fe2+ 和 Ox 各自的作用。此外，还研究了螯合剂和水基质对紫外/Fe2+/Ox 降解 NOR 的影响。紫外/Fe2+/Ox 工艺在实际水体中显示出令人满意的 NOR 降解效果，表明其具有实际应用潜力。新型紫外/Fe2+/氧化工艺对 NOR 的降解大大降低了其对环境和健康的危害。

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来源期刊

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.