摘要
有机磷酸酯(OPEs)作为备受关注的一类新污染物,已对偏远的南极地区水环境引发了中等风险.磷酸三苯酯(TPHP)是水体中常见的OPEs,已被证实具有毒性效应、生物富集和放大效应,对环境和人体健康威胁较大.利用傅里叶红外光谱仪(FT-IR)和液相色谱-串联质谱联用仪(LC-MS/MS)探究TPHP在紫外-过氧化氢(UV-H_(2)O_(2))、紫外-二氧化钛(UV-TiO_(2)_(2))和紫外-过硫酸盐(UV-PS)这3种高级氧化体系(UV-AOPs)中的降解过程,创新性地利用FT-IR实现了TPHP降解过程中红外特征峰变化的在线观测,并对其降解反应动力学、光降解产物和降解路径进行了分析.结果表明,TPHP在UV-H_(2)O_(2)、 UV-TiO_(2)和UV-PS体系下均能得到有效降解,其光降解半衰期分别为74、 150和89 min.其中,UV-H_(2)O_(2)体系对TPHP的降解效果最好. TPHP在3种体系下的降解反应均符合一级动力学.当H_(2)O_(2)浓度为0~0.097 mol·L^(-1)时,H_(2)O_(2)浓度升高会促进TPHP降解;当TiO_(2)浓度为0~0.013 mol·L^(-1)时,TiO_(2)浓度升高会促进TPHP降解. TPHP的光降解路径主要是P—O—C键断裂、苯环结构的C—H键断裂和水解反应.利用UV-H_(2)O_(2)体系对成都市环境水体中OPEs进行降解实验,发现对公园景观水体的水样进行降解反应60 min时,TPHP的去除率为66%.
As a type of emerging pollutant of concern, organophosphate esters(OPEs) have posed a moderate risk to the remote Antarctic waters. Triphenyl phosphate(TPHP) is a common type of OPEs in water, which has been proven to have toxic effects, bioaccumulation, and amplification effects and pose a great threat to the environment and human health. Fourier transform infrared spectroscopy(FT-IR) and liquid chromatography-tandem mass spectrometry(LC-MS/MS) were used to investigate the degradation process of TPHP in three advanced oxidation processes(UV-AOPs), including ultraviolet-hydrogen peroxide(UV-H_(2)O_(2)), ultraviolet-titanium dioxide(UV-TiO_(2)), and ultraviolet-persulfate(UV-PS) systems. This was the first instance of using FT-IR for the online observation of the change in infrared characteristic peaks in the degradation process of TPHP, and its degradation reaction kinetics, photodegradation products, and degradation pathways were analyzed. The results showed that TPHP could be effectively degraded under UV-H_(2)O_(2), UV-TiO_(2), and UV-PS systems, and the photodegradation half-lives were 74, 150, and 89 min, respectively. The UV-H_(2)O_(2)system had the best degradation effect on TPHP. Additionally, the degradation reactions of TPHP in three systems conformed to the first-order kinetics. When the concentration of H_(2)O_(2)was 0-0.097 mol·L^(-1), the increase in H_(2)O_(2)concentration promoted the degradation of TPHP, and when the concentration of TiO_(2)was 0-0.013 mol·L^(-1), the increase in TiO_(2)concentration promoted the degradation of TPHP. The photodegradation pathway of TPHP mainly included the P—O—C bond breaking, the C—H bond cleavage of the benzene ring structure and the hydrolysis reaction of TPHP. The UV-H_(2)O_(2)system was used to degrade OPEs in the environmental water of Chengdu, and it was found that the removal rate of TPHP was 66% when the water samples of the park landscape water were degraded for 60 min.
作者
徐子文
印红玲
熊远明
宋娇娇
谯炀
XU Zi-wen;YIN Hong-ling;XIONG Yuan-ming;SONG Jiao-jiao;QIAO Yang(College of Resources and Environment,Chengdu University of Information Technology,Chengdu 610225,China)
出处
《环境科学》
EI
CAS
CSCD
北大核心
2022年第11期4992-4999,共8页
Environmental Science
基金
国家自然科学基金项目(41773072)。
关键词
磷酸三苯酯
降解
紫外高级氧化
反应动力学
半衰期
triphenyl phosphate
degradation
ultraviolet advanced oxidation process
reaction kinetics
half-life
