【作者】 胡淼；

【导师】 徐向阳；

【作者基本信息】 浙江大学 ， 环境工程（专业学位）， 2016， 硕士

【摘要】 近年来,内分泌干扰物(EDCs)等新型有机物污染问题日益凸显,我国多处地表水和污水处理厂出水中EDCs含量达几十μg·L-1甚至更高,表明现有污水处理工艺不能有效去除上述EDCs.含EDCs污水排入受纳水体严重威胁生态环境安全和居民饮水健康,因此,探寻经济有效的EDCs污水处理工艺技术具有重要现实意义。论文以典型类固醇雌激素为研究对象,应用傅里叶红外光谱(FTIR)、液相色谱-质谱联用(LC/MS)、高通量测序等技术,开展了絮体污泥与好氧颗粒污泥去除典型雌激素的过程特性、处理含典型雌激素城镇污水好氧颗粒污泥污泥工艺性能等研究,取得如下主要研究结果：1、研究絮体污泥和好氧颗粒污泥对典型类固醇雌激素的吸附特性发现,雌激素在絮体污泥和好氧颗粒污泥上的吸附规律相似,在初始雌激素浓度250μg·L-1～40000μg·L-1条件下吸附在4h达到平衡,吸附等温线较好符合Langmuir方程和Freundlich方程,相关系数R2分别为0.924～0.959和0.949～0.975。其中,好氧颗粒污泥对典型类固醇雌激素E2、EE2的吸附过程与准二级动力学拟合较好(R2>0.992),表明好氧颗粒污泥吸附E2、EE2是以化学吸附为主的物理-化学吸附过程。研究还发现,污泥浓度、pH、温度等影响雌激素吸附性能。2、研究絮体污泥和好氧颗粒污泥对E2、EE2的生物降解性能,结果表明,在初始浓度4000μg·L-1条件下,絮体污泥和好氧颗粒污泥对E2的去除率均在94%以上,其中生物降解所占比例分别为66.5%、68.8%,表明E2去除以生物降解为主；絮体污泥和颗粒污泥对EE2的去除率分别为75.5%、88.9%,其中吸附所占比例分别为67.1%和69.3%,表明EE2去除以吸附为主。结合不同结构污泥显微观察发现,好氧颗粒污泥较大的比表面积与丰富的氨基、羟基、羧基等表面化学官能团有利于雌激素的吸附与功能微生物的附着。3、启动SBR好氧颗粒污反应器研究雌激素去除效能,结果表明,颗粒污泥反应器在进水COD、TN、E2/EE2负荷分别为1.5kg·m-3·d-1、0.08kg·m-3·d-1、 0.03g·m-3·d-1条件下运行120d,颗粒污泥平均粒径达685±±35μm,系统MLSS、SVI分别稳定在5.8±0.1g·L-1、34mL·g-1, COD、NH4+-N、TN去除率分别稳定在94.6%±0.2%、97.5%±0.1%、73.5%±0.3%,E2、EE2去除率则达88.6±0.7%和73.2±0.5%,表明好氧颗粒污泥工艺对雌激素具有良好的去除效能。分析反应器运行过程污泥微生物菌群结构变化发现,处理含雌激素污水的R1反应器运行90d,Shannon指数从3.58上升到5.65,菌群丰富度提高。颗粒污泥主要优势菌群为Proteobacteria和Actinobacteria,其丰度分别为60.1%和27.2%。对比对照组R2,R1污泥Sphingomonas spp.丰度由1.02%增至13.9%,Pseudomonas spp.由1.02%增至13.2%,分析认为这两种菌属对雌激素物质降解有重要作用。研究结果初步揭示好氧颗粒污泥工艺去除雌激素的微生物学机制。更多还原

【Abstract】 In recent years, new types of organic pollutants such as endocrine disrupting chemicals (EDCs) have become a rising challenge in wastewater treatment. Researches show that the concentration of EDCs in surface water and sewage treatment plant effluents had reached dozens of μg·L-1 or even higher. These pollutants cannot be removed effectively through traditional methods.It’11 be a big threat to ecological environment and drinking water safety when the EDCs are discharged into receiving water body. Therefore, it’s of great significance to search for economical and effective techniques for EDCs removal. This thesis focused on typical steroid estrogens, the characteristics of removal process by floc sludge and aerobic granular sludge and the performance of aerobic granular sludge process treating steroid wastewater containing estrogens were studied with the application of FTIR, LC/MS and high-throughout sequencing technique. Main conclusions are as follows:1. Study on the adsorption characteristics of estrogens by floc sludge and aerobic granular sludge were performed via batch tests. Results showed the adsorption process of estrogen by floc sludge and aerobic granular sludge were similar. Adsorption equilibrium was reached after 4 hours when the initial estrogen concentration was at 250 μg·L-1～4000μg·L-1. The adsorption isotherm was followed by Langmuir equation and Freundlich equation with the correlation coefficients at 0.924-0.959 and 0.949-0.975, respectively. Adsorption process of E2 and EE2 by aerobic granular sludge was followed with pseudo-second order kinetic with R2>0.992, indicating this process was a physical and chemical process where chemical adsorption was the major role. MLSS, pH and temperature were all the crucial factors on estrogens adsorption.2. Study on adsorption and degradation process of E2 and EE2 showed that with the initial concentration of 4mg·L-1, E2 removal efficiencies by floc and aerobic granular sludge were above 94%, among which biological degradation percentages were at 66.5% and 68.8%, respectively. Results showed that E2 was mainly removed by biological degradation. EE2 removal efficiencies by floc and aerobic granular sludge were 75.5% and 88.9%, among which adsorption percentages were 67.1% and 69.3%, respectively. Results showed that EE2 was mainly removed by adsorption degradation.Results of SEM and FTIR showed that the core structureand large surface aera and complexation reaction of chemical functional groups (amino, hydroxyl radical, carboxyl) of aerobic granular sludge favor the adsorption and microbial enrichment.3.In order to test the efficacy of aerobic granular sludge to remove estrogens. reactors were set up with influent COD, NH4+-N and E2/EE2 concentration of 1.5kg·m-3·d-1,0.08·kg·m-3d-1 and 0.03·g·m-3-d-1.Mean diameter of aerobic granular sludge after 120d running reached 685±35μm, while MLSS and SVI were at 5.8±0.1g·-L-1 and 34ml·g-1, respectively. COD, TN and NH4+-N efficiency were 94.6±0.2%,73.5±0.3% and 97.5±0.1%. Meanwhile, E2 and EE2 removal were 88.6±0.7% and 73.2±0.5%, confirming that aerobic granular sludge removed estrogens effectively.Results of microbial community succession showed that the shannon index of granular sludge reactor increased from 3.58 to 5.65. Compared to regular reactor R2, Proteobacteria and Actinobacteria were dominant microbies in R1 reactor with a proportion of 60.1% and 27.2%. At the same time, Sphingomonas spp. increased from 1.02% to 13.50%, and Pseudomonas spp. increased from 0.02% to 10.38%. It’s speculated that these two strains are important in estrogen degradation.The results reveal the microorganism mechanism of estrogen degradation by aerobic granular sludge.更多还原