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介电阻挡放电等离子体(DBDP)与过硫酸盐(PS)氧化体系联合降解河流沉积物中莠去津:响应面法、降解机制和途径。

Degradation of atrazine in river sediment by dielectric barrier discharge plasma (DBDP) combined with a persulfate (PS) oxidation system: response surface methodology, degradation mechanisms, and pathways.

机构信息

School of Biology, Food, and Environment, Hefei University, No. 99 Jinxiu Road, Hefei, 230601, China.

Heifei Engineering Research Center for Soil and Groundwater Remediation, Hefei, 230088, China.

出版信息

Environ Sci Pollut Res Int. 2023 Apr;30(17):51303-51313. doi: 10.1007/s11356-022-24927-0. Epub 2023 Feb 21.

DOI:10.1007/s11356-022-24927-0
PMID:36809616
Abstract

Single degradation systems based on dielectric barrier discharge plasma (DBDP) or persulfate (PS) oxidation cannot achieve the desired goals (high degradation efficiency, high mineralization rate, and low product toxicity) of degrading atrazine (ATZ) in river sediment. In this study, DBDP was combined with a PS oxidation system (DBDP/PS synergistic system) to degrade ATZ in river sediment. A Box-Behnken design (BBD) including five factors (discharge voltage, air flow, initial concentration, oxidizer dose, and activator dose) and three levels (- 1, 0, and 1) was established to test a mathematical model by response surface methodology (RSM). The results confirmed that the degradation efficiency of ATZ in river sediment was 96.5% in the DBDP/PS synergistic system after 10 min of degradation. The experimental total organic carbon (TOC) removal efficiency results indicated that 85.3% of ATZ is mineralized into CO, HO, and NH, which effectively reduces the possible biological toxicity of the intermediate products. Active species (sulfate (SO•), hydroxy (•OH), and superoxide (•O) radicals) were found to exert positive effects in the DBDP/PS synergistic system and illustrated the degradation mechanism of ATZ. The ATZ degradation pathway, composed of 7 main intermediates, was clarified by Fourier transform infrared spectroscopy (FTIR) and gas chromatography-mass spectrometry (GC-MS). This study indicates that the DBDP/PS synergistic system is a highly efficient, environmentally friendly, novel method for the remediation of river sediment containing ATZ pollution.

摘要

基于介质阻挡放电等离子体(DBDP)或过硫酸盐(PS)氧化的单一降解系统无法实现降解河流沉积物中莠去津(ATZ)的预期目标(高降解效率、高矿化率和低产物毒性)。在本研究中,DBDP 与 PS 氧化系统(DBDP/PS 协同系统)结合用于降解河流沉积物中的 ATZ。采用 Box-Behnken 设计(BBD),包括五个因素(放电电压、空气流量、初始浓度、氧化剂剂量和活化剂剂量)和三个水平(-1、0 和 1),通过响应面法(RSM)建立数学模型进行测试。结果证实,在 10 分钟的降解后,DBDP/PS 协同系统中河流沉积物中 ATZ 的降解效率达到 96.5%。实验总有机碳(TOC)去除效率结果表明,85.3%的 ATZ 矿化为 CO、HO 和 NH,有效降低了中间产物可能的生物毒性。发现活性物质(硫酸盐(SO•)、羟基(•OH)和超氧自由基(•O))在 DBDP/PS 协同系统中发挥了积极作用,并说明了 ATZ 的降解机制。通过傅里叶变换红外光谱(FTIR)和气相色谱-质谱(GC-MS)阐明了由 7 种主要中间体组成的 ATZ 降解途径。本研究表明,DBDP/PS 协同系统是一种高效、环保、新颖的修复含有 ATZ 污染的河流沉积物的方法。

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