中文版 | English
Title

华南与华北典型城市水环境抗生素分布特征与光催化降解研究

Alternative Title
RESEARCH ON ANTIBIOTIC DISTRIBUTION CHARACTERISTICS AND PHOTOCATALYTIC DEGRADATION IN WATER ENVIRONMENT OF TYPICAL CITIES IN SOUTH AND NORTH CHINA
Author
Name pinyin
FU Caixia
School number
11849589
Degree
博士
Discipline
0830 环境科学与工程
Subject category of dissertation
08 工学
Supervisor
郑春苗
Mentor unit
环境科学与工程学院
Publication Years
2022-05-16
Submission date
2022-07-11
University
哈尔滨工业大学
Place of Publication
哈尔滨
Abstract

广泛使用抗生素治疗人类、动物和植物感染性疾病,导致水环境中抗生素污染严重,且对公众健康和水生生物构成潜在威胁。因此,抗生素污染问题在世界范围内受到高度关注。本研究旨在调查我国华南、华北两座重要城市的40种抗生素的污染特征,评估抗生素的水环境生态风险,并在此基础上开发高效降解环境浓度抗生素的光催化技术。华南、华北区域内的两座城市由于气候和经济发展水平不同,抗生素的污染种类、浓度和时空分布特点存在差异,通过对比两市抗生素分布特征,可以更加系统全面揭示不同地域条件下抗生素在不同环境介质中的迁移转化规律,为我国抗生素的污染防治提供数据与理论支撑。

针对华南地区某市夏季和冬季的地下水样品中40种抗生素的检出、季节分布和生态风险等展开研究。抗生素的总浓度范围分别为夏季34.73~1344.17 ng/L,冬季1.39~633.84 ng/L,夏季地下水抗生素污染浓度高于冬季。夏季降雨量增加,地表水地下水交换作用更强,水溶性较强更容易迁移的抗生素在地下水中含量增高,例如磺胺对甲氧嘧啶(检出率:40.32%)和磺胺甲恶唑(检出率:50%)在地下水中含量较高,浓度分别为~123.61 ng/L和~253.07 ng/L。研究表明磺胺甲基嘧啶、磺胺甲二唑、诺氟沙星、环丙沙星和达氟沙星等抗生素对抗性基因(Antibiotic Resistance Genes,ARGs)扩散有显著促进作用。此外,SO42-、F-、TDS、DO和pH等水质参数对ARGs扩散的促进作用也不容忽视。

华北地区某市水环境中地表水、地下水和沉积物中抗生素污染浓度范围分别为12.71~260.56 ng/L、~196.12 ng/L和38.03~406.31 ng/g。在地表水和沉积物中,头孢菌素类和喹诺酮类是主要检出抗生素,在地表水中分别占抗生素总浓度的45%和16%,在沉积物中分别占总抗生素浓度的62%和32%,这一结果表明两种介质之间存在重要的交互转化作用。在<50 m深度的浅层地下水中抗生素浓度最高(平均浓度为79.22±56.46 ng/L),表明地表水是地下水中抗生素污染的主要来源。阿莫西林和磺胺甲恶唑在地表水和地下水中的风险较高,应作为优先控制抗生素。此外,在华北某市的沉积物中发现了抗生素对ARGs的选择压力,因为sulA的富集与螺旋霉素和林可霉素显著相关,而blaOXA-1的富集与罗红霉素、环丙沙星、氧氟沙星和磺胺吡啶显著相关。

本研究采用光催化氧化法降解两城市均需优先控制的抗生素磺胺甲恶唑,选用廉价易得、无毒、稳定性高的市售二氧化钛(TiO2)作为催化剂,选用可产生多样化活性基团的强还原性含硫化合物连二亚硫酸钠(DTN,S2O42-)作为自由基产生源。研究结果表明使用TiO2作为催化剂活化DTN实现了磺胺甲恶唑的高效降解。在TiO2/DTN体系中,1 h内便可实现磺胺甲恶唑100%的高效去除。通过探究催化剂用量和DTN浓度对降解效率的影响,最终确定最优化反应条件TiO2投加量为5 mg,DTN与磺胺甲恶唑摩尔比为20:1。磺胺甲恶唑可以在碱性条件(pH为7.0~11.0)下被高效的去除,在酸性条件(pH为1.0~5.0)下受到显著的抑制。在碳酸氢根的存在下,磺胺甲恶唑的降解基本不受影响,浓度50~200 mg/L时有促进作用。但是在硝酸根,氯离子和腐殖酸的存在下,磺胺甲恶唑的降解则会受到显著的抑制,抑制作用随着浓度增加而增加。通过自由基淬灭和捕获实验,证明了主要活性基团为硫酸根自由基、羟基自由基和单线态氧。

Keywords
Language
Chinese
Training classes
联合培养
Enrollment Year
2018
Year of Degree Awarded
2022-07
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Academic Degree Assessment Sub committee
环境科学与工程学院
Domestic book classification number
X52/X826
Data Source
人工提交
Document TypeThesis
Identifierhttp://kc.sustech.edu.cn/handle/2SGJ60CL/353273
DepartmentSchool of Environmental Science and Engineering
Recommended Citation
GB/T 7714
付彩霞. 华南与华北典型城市水环境抗生素分布特征与光催化降解研究[D]. 哈尔滨. 哈尔滨工业大学,2022.
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