典型人工甜味剂在深圳近海岸水体中的归趋特征研究

RESEARCH ON THE FATE OF TYPICAL ARTIFICAL SWEETENERS IN OFFSHORE WATER OF SHENZHEN

刘庆伟

11849174

硕士

环境工程

郭伟

2020-05-28

2020-06-10

哈尔滨工业大学

深圳

人工甜味剂（ASs）是一类蔗糖替代物，其作为添加剂被大量使用。近期研究表明，人工甜味剂具有生态毒性效应且在污水处理厂（WWTPs）和天然水体环境中大量赋存，这使其成为一种新型污染物质并对生态系统造成威胁，因此这类物质在污水处理厂及受纳水体中的归趋特征亟待研究。本研究选取安赛蜜、甜蜜素、糖精、三氯蔗糖、阿斯巴甜和纽甜6种人工甜味剂，通过建立并优化出一套前处理和仪器分析方法，实地调查了深圳4座污水处理厂及受纳水体，定量评估了污水处理厂输入和排放的人工甜味剂的污染贡献，综合分析了人工甜味剂的归趋特征。建立了人工甜味剂的前处理方法和仪器分析方法。水样的分析方法为固相萃取+高效液相色谱串联质谱分析（HPLC-MS/MS），方法检出限为0.4 ng/L～51.8 ng/L，定量限为1.4 ng/L～172.8 ng/L，回收率为90%～123%；固体样品的分析方法为超声萃取+固相萃取+HPLC-MS/MS，方法检出限为0.8 ng/g～43.2 ng/g，定量限为2.7 ng/g～144.0 ng/g，回收率为54%～94%。该方法能够满足痕量分析需求。选取深圳4座近海岸污水处理厂及受纳水体进行实地调查。结果表明，水样中6种人工甜味剂全部检出，浓度为nd（未检出）～35.23 μg/L；悬浮颗粒物中检出安赛蜜、甜蜜素、阿斯巴甜和纽甜，浓度为nd～65.97 μg/g；污泥中检出甜蜜素、纽甜和阿斯巴甜，浓度为0.04 μg/g～0.20 μg/g。安赛蜜、糖精、甜蜜素、三氯蔗糖在污水厂中的去除率很高（80.31%～100%），阿斯巴甜在WWTP1中难以去除（0.02%）而在WWTP2中去除率很高（85.11%），纽甜则难以去除（0.97%～13.76%）。研究还分析了水质参数对人工甜味剂分布特征的影响，污水厂中溶解性有机碳浓度（DOC）是关键影响参数，受纳水体中氧化还原电位（ORP）和254 nm紫外吸光度（UV254）是关键影响参数，阿斯巴甜和纽甜更容易在污泥和颗粒相中赋存。定量分析了人工甜味剂在污水处理厂的输入和排放特征。其中，三氯蔗糖和糖精的平均输入负荷（0.76 g/d/1000 people～7.62 g/d/1000 people、0.86 g/d/1000 people～4.65 g/d/1000 people）最大，纽甜的平均输入负荷（0.02 g/d/1000 people）最小。WWTP1、WWTP2中阿斯巴甜和三氯蔗糖的平均排放负荷（0.04 g/d/1000 people～0.05 g/d/1000 people、0.04 g/d/1000 people～1.28 g/d/1000 people）最大，WWTP3、WWTP4中安赛蜜的平均排放负荷（0.24 g/d/1000 people～0.28 g/d/1000 people）最大，本研究的平均输入和排放负荷普遍小于国外。

Artificial sweeteners (ASs) are substitutes for sucrose, which are widely used as additives. Recent studies have shown that ASs have eco-toxic effects and are abundant in wastewater treatment plants (WWTPs) and water environments. As a kind of emerging organic pollutant which will threaten ecosystems, the fate of ASs in WWTPs and receiving water need to be studied urgently. In this study, six ASs including acesulfame, cyclamate, saccharin, sucralose, aspartame, and neotame were investigated in four WWTPs and receiving waters near coast of Shenzhen city based on the optimized pretreatment and instrumental analysis methods. Pollution contribution of input and output artificial sweeteners in WWTPs was quantitatively evaluated, and comprehensively analyzed the fate of artificial sweeteners.The pretreatment and instrument analysis methods of ASs were established. The analysis method of water samples was solid phase extraction combined with high-performance liquid chromatography and mass spectrometry (HPLC-MS/MS). The detection limit was 0.4 ng/L-51.8 ng/L, and the limit of quantification was 1.4 ng/L-172.8 ng/L, the recovery rate was 90%-123%. The analysis method of solid sample was ultrasonic extraction combined with water sample analysis method. The detection limit was 0.8 ng/g-43.2 ng/g, the limit of quantification was 2.7 ng/g-144.0 ng/g, and the recovery rate was 54%-94%. This method can meet the demands of trace analysis.Water and solid phase samples from coastal WWTPs and their receiving waters in Shenzhen city were investigated. The results showed that all ASs were detected in water samples, with a concentration of nd(not detected)-35.23 μg/L. Acesulfame, cyclamate, aspartame, and neotame were easily detected in suspended particles, with a concentration of nd-65.97 μg/g. Cyclamate, neotame and aspartame were detected in the sludge, with a concentration of 0.04 μg/g-0.20 μg/g. The removal rate of acesulfame, saccharin, cyclamate, and sucralose in four WWTPs was very high (80.31%-100%), and aspartame was difficult to remove in WWTP1(0.02%) but had a high removal rate in WWTP2 (85.11%), and neotame was difficult to remove (0.97%-13.76%). Futhermore, the influence of water quality characteristics on the distribution of ASs was evaluted. The concentration of dissolved organic carbon (DOC) was the key influencing factor for the distribution of ASs in WWTPs. The oxidation reduction potentia (ORP) and ultraviolet absorbance at 254 nm (UV254) were the key influencing parameters for the distribution of ASs in receiving waters. Aspartame and neotame were more likely to exist in sluge and particle phase.The input and output loads of ASs in WWTPs were quantitatively analyzed. Among them, the average input load of sucralose and saccharin (0.76 g/d/1000 people-7.62 g/d/1000 people, 0.86 g/d/1000 people-4.65 g/d/1000 people) was the largest, and the average input load of neotame (0.02 g/d/1000 people) was the smallest. The average output load of aspartame and sucralose in WWTP1 and WWTP2 (0.04 g/d/1000 people-0.05 g/d/1000 people, 0.04 g/d/1000 people-1.28 g/d/1000 people) was the largest. The average output load of acesulfame in WWTP3 and WWTP4 (0.24 g/d/1000 people-0.28 g/d/1000 people) was the largest. Moreover, the average input and output loads of ASs in these WWTPs were smaller than that in WWTPs from foreign countries.

人工甜味剂 近海岸 污水处理厂 归趋 悬浮颗粒物 污染负荷

artificial sweetener offshore water wastewater treatment plants fate suspended particle pollution load

中文

联合培养

南方科技大学

刘庆伟. 典型人工甜味剂在深圳近海岸水体中的归趋特征研究[D]. 深圳. 哈尔滨工业大学,2020.