UV_(254)/NH_(2)Cl体系降解水中新污染物的反应动力学与产物预测  

UV_(254)/NH_(2)Cl System for Degradation of Emerging Pollutants in Water:Reaction Kinetics and Product Prediction

作　　者：蒋雅茵 石美燕 刘梦霏 孙启元[1,3] 王菲凤 蔡开聪[2] JIANG Yayin;Shi Meiyan;LIU Mengfei;SUN Qiyuan;WANG Feifeng;CAI Kaicong(College of Environmental and Resource Sciences,College of Carbon Neutral Modern Industry,Fujian Normal University,Fuzhou 350117,China;College of Chemistry and Materials Science,Fujian Normal University,Fuzhou 350117,China;Fujian Key Laboratory of Pollution Control&Resource Reuse,Fuzhou 350117,China;Fuzhou Water Quality Monitoring Co.,Ltd,Fuzhou 350007,China)

机构地区：[1]福建师范大学环境与资源学院、碳中和现代产业学院,福州350117 [2]福建师范大学化学与材料学院,福州350117 [3]福建省污染控制与资源循环利用重点实验室,福州350117 [4]福州水质监测有限公司,福州350007

出　　处：《亚热带资源与环境学报》2025年第1期81-89,共9页Journal of Subtropical Resources and Environment

基　　金：国家自然科学基金项目(52070044);福建自然科学基金项目(2021J06022)。

摘　　要：紫外线联合氯胺(UV_(254)/NH_(2)Cl)工艺是一种前景广阔的高级氧化工艺(AOP),该工艺能产生多样活性物种协同高效去除水中新有机污染物。本研究以9,10-二氢-9-氧杂-10-磷杂菲-10-氧化物(DOPO)、磷酸氯喹(CP)、避蚊胺(DEET)为目标污染物,探讨了UV_(254)/NH_(2)Cl对这些新污染物的降解动力学,阐析了水质条件和工艺参数对降解过程的影响,并通过Fukui指数计算,分析了3种污染物分子结构在降解反应过程中易被攻击而断裂的键位及降解产物与毒性。结果表明,相较于单一UV、NH_(2)Cl体系,UV_(254)与NH_(2)Cl联用对3种污染物的表观降解速率常数(k obs)分别提升3.2、3.8、7.3倍,在UV_(254)/NH_(2)Cl体系中,随着NH_(2)Cl用量的增加,3种污染物的降解速率随之提升。当NH_(2)Cl的用量从0增到300μmol·L^(-1)时,k obs从6.86×10^(-5)s^(-1)上升到5.67×10^(-4)s^(-1)。水中不同pH对DOPO的降解影响表现为,当pH从4.0增加到7.0时,DOPO的降解率下降了9%,而当pH从7.0增加到9.0时,DOPO的降解率提高,这可能与氯胺的氧化性能、紫外光激发效应及DOPO的分子结构性质有关。综上所述,UV/NH_(2)Cl体系能降低DOPO、CP、DEET等多种新有机污染物在水体中的含量及毒性,可以为污水净化提供一种新思路与方法。The ultraviolet-254 nm combined with chloramine(UV_(254)/NH_(2)Cl)process is a promising advanced oxidation process(AOP)that generates a variety of reactive species for the efficient removal of emerging organic contaminants pollutants from water.This study investigates the degradation kinetics of 9,10-Dihydro-9-oxa-10-phosphaphenanthrene-10-oxide(DOPO),chloroquine phosphate(CP)and mosquito avoidance amine(DEET)by the UV_(254)/NH_(2)Cl system,elucidating the impact of water quality conditions and process parameters on the degradation process.Additionally,Fukui index calculations were employed to analyze the susceptible bond positions in the molecular structures of these three pollutants that are prone to attack and break during the degradation reaction,as well as the degradation products and their toxicity.Results indicated that the apparent degradation rate constants(k obs)for the three pollutants were enhanced by 3.2,3.8 and 7.3 times,respectively,when UV_(254)is combined with NH_(2)Cl compared to using UV or NH_(2)Cl alone.In the UV_(254)/NH_(2)Cl system,the degradation rate of the three pollutants accelerated with the increasing addition dosage of NH_(2)Cl.Specifically,as the NH_(2)Cl dosage increased from 0 to 300μmol·L^(-1),k _(obs) rose from 6.86×10^(-5)s^(-1)to 5.67×10^(-4)s^(-1).The effect of different pH levels on the degradation of DOPO in water showed that as pH value increased from 4.0 to 7.0,the degradation rate of DOPO decreased by 9%,while pH value increased from 7.0 to 9.0,the degradation rate of DOPO increased.This may be related to the oxidizing properties of NH_(2)Cl,the excitation effect of UV light,and the molecular structure characteristics of DOPO.In summary,the UV_(254)/NH_(2)Cl system can reduce the content and toxicity of various organic pollutants,such as DOPO,CP,DEET in water,providing a new perspective and method for waste water purification.

关 键 词：UV 254/NH 2Cl 反应动力学 高级氧化技术 新有机污染物 降解产物 

分 类 号：X703.1[环境科学与工程—环境工程]