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题名: 饮用水输配过程中管网稳定性与消毒副产物控制研究
作者: 胡俊1
学位类别: 博士
答辩日期: 2017-05
授予单位: 中国科学院大学
授予地点: 北京
导师: 强志民
关键词: 管网腐蚀产物,消毒副产物,过一硫酸盐消毒,VUV/UV,铁释放 ; Pipe corrosion products ; Disinfection by-products ; PMS disinfection ; VUV/UV ; Iron release
其他题名: Stability of drinking water distribution systems and control of disinfection by-products
学位专业: 环境工程
中文摘要: 在输配过程中,自来水与管道内壁表面之间发生了极其复杂的物理、化学和 生物反应,可能造成管网供水的“二次污染”。本文中试规模研究了管网水质对 管垢和微生物的影响;为了保持管网生物的稳定性,自由氯是应用最广泛的消毒 剂,研究了典型氯消毒过程中三种铜腐蚀产物(CCPs,包括 CuO、Cu2O和 Cu2+) 对溴酸根(BrO3−)和溴代消毒副产物(Br-DBPs)同时生成的催化作用;针对氯 消毒管网中大量产生消毒副产物的问题,提出以过一硫酸盐(PMS)作为消毒剂, 并研究了在 PMS消毒过程中两种管道腐蚀产物(PCPs,包括 CuO和 δ-MnO2) 对碘帕醇(IPM)转化的催化作用;针对碘代消毒副产物(I-DBPs)的生成的问 题,提出在二次供水或者供水终端采用真空紫外( VUV/UV)技术,并研究了 VUV/UV技术对三种 I-DBPs(CHI3、CHI2CONH2和 CI3COOH)的降解。 与以地表水为水源的管段(P2)相比,以地下水为水源的管段(P3)铁释放 较为剧烈。高浓度的 Cl–和 SO42–促进了管段的铁释放,而碱度和硬度的增加减缓 管段的铁释放。此外,将消毒剂由氯切换成氯胺也可以控制管段铁释放。DO的 消耗与铁释放具有较好的相关性。铁释放越激烈,DO的消耗越大。管垢的主要 的晶体铁氧化物为磁铁矿(Fe3O4)和针铁矿(α-FeOOH),此外含有少量的纤铁 矿(γ-FeOOH)和四方纤铁矿(β-FeOOH)。P2中 Fe3O4/α-FeOOH值比 P3中的 Fe3O4/α-FeOOH值大,说明 P2中的管垢更加稳定。随着反应器的运行, Fe3O4/α-FeOOH值基本保持不变。碱度和钙硬度的增加导致 FeCO3和 CaCO3生 成,减缓铁的释放。水质严重影响着管垢中的微生物群落,中试过程中 SOB、 SRB和 IOB的含量大幅增加,而 IRB的含量基本不变。 CCPs可以大幅度催化 Br-DBPs和 BrO3−的生成,而腐殖酸(HA)的存在大 幅度抑制了 BrO3−的催化生成。在 HOCl/Br−/CuO系统中,CuO主要促进 BrO3− 的生成;而在 HOCl/Br−/Cu2O和 HOCl/Br−/Cu2+系统中,Cu2O和 Cu2+主要促进 Br-DBPs的生成。pH重要影响着 CCPs对 Br-DBPs和 BrO3−生成的催化作用。随 着 pH增大,CCPs对 Br-DBPs的催化作用增强。然而,CCPs对 BrO3−生成的催 化作用在 pH7.6时达到最大;随着 CCPs剂量的增加,Cu2O与 Cu2+的对 Br-DBPs 催化效果大幅度加强,而 CuO对 BrO3−的催化效果大幅度加强。随着 Br−初始浓 度的增加,CCPs对 BrO3−生成的催化作用增强,而对 Br-DBPs的催化作用并未加强。水体基质(例如,有机成分和无机离子)重要影响着 CCPs对 Br-DBPs和BrO3−生成的催化作用。 CuO/PMS体系(CuPS)中 IPM的降解速率是 δ-MnO2/PMS(MnPS)中 IPM 降解速率的 3.7倍,分别为 0.218和 0.059 min–1。在 CuPS中 SO4•−是 IPM降解的 主要贡献者,而在 MnPS中 HO•对 IPM降解也具有重要作用。CuPS和 MnPS中 自由基的产率分别为 0.89和 0.69 mol/mol。在 CuPS和 MnPS中,IPM的降解速 率在 PCPs剂量分别为 1.5和 1.0 g L–1时达到最大。IPM的降解速率随着 PMS剂 量增大而增大。IPM的降解率在 pH7时达到最大。水体基质(NOM、碱度和 Cl–) 对 IPM的降解有不同程度的抑制作用。IPM中释放的碘素大部分被氧化为 IO3–, 而只有少量的碘素转化为 CHI3。PMS消毒过程中 IPM的转化主要通过两个途径: 1)支链 A中酰基的水解、氨基的氧化和支链 B与 B’中酰基的水解;2)脱碘反 应。与 UV辐照相比,VUV/UV辐照能更好地去除 I-DBPs。三种 I-DBPs的去除 效果依次为:CHI3>CHI2CONH2>CI3COOH。在 VUV/UV辐照的过程中,UV是 I-DBPs降解的主要贡献者。三种 I-DBPs发生逐步脱碘反应,在 UV辐照下只生 成 I‒,而在 VUV/UV辐照下,部分 I‒被 HO•氧化成 IO3‒。在 UV辐照下,三种 I-DBPs的降解速率随着 pH的增大而增大,而在 VUV/UV的辐照下,三种 I-DBPs 的降解速率随着 pH的增大而减小。UV和 VUV/UV辐照下,水体基质(NOM、 HCO3‒和 Cl–)对三种 I-DBPs的降解有不同程度的抑制作用。 本文研究了管网水质对管垢及微生物群落稳定性的影响、管网腐蚀产物对消 毒物副产物生成的影响以及二次供水或终端供水中消毒副产物的去除,将有助于 控制消毒副产物的生成和管垢金属的释放,预防管网供水的“二次污染”,保证 输配过程中饮用水水质的安全与健康。
英文摘要: In drinking water distribution systems (DWDSs), bulk water interacts with the pipe inner-surface through physical, chemical and biological reactions, resulting in the “secondary pollution”. This study determined the influence of water quality on the corrosion scales and bacterial community in cast iron pipes for water distribution at pilot-scale. To maintain the stability of microorganism in the DWDSs, free chlorine is the most widely used disinfectant. The study investigated the catalysis of three different copper corrosion products (CCPs, including CuO, Cu2O and Cu2+) on the simultaneous formation of bromate (BrO3−) and bromated disinfection by-products (Br-DBPs) during chlorination of Br−-containing waters. In view of the considerable formation of DBPs during chlorination in DWDSs, peroxymonosulfate (PMS) was adopted as an alternative disinfectant. The iopamidol (IPM) degradation by PMS under catalysis of two pipe corrosion products (PCPs, including CuO and δ-MnO2) was studied. The vacuum ultraviolet (VUV) technology was applied during the secondary or terminal water supply to remove iodinated disinfection by-products (I-DBPs). The degradation of I-DBPs under UV and VUV/UV irradiation was investigated. The iron release in pipes (P2) transporting surface water was slower than that in the pipes transporting groundwater (P3) during the operation period. The increase of Cl− and SO42− concentration accelerated the iron release, while the augment of alkalinity and calcium hardness inhibited the iron release. The disinfectant shifted from FC to MC slightly retarding the iron release. The dissolved oxygen consumption (ΔDO) was highly relative to the iron release in the three pipes. Magnetite (Fe3O4) and goethite (α-FeOOH) were the main crystalline iron minerals in the three pipes. The other iron oxides, such as lepidocrocite (γ-FeOOH) and akaganeite (β-FeOOH), were also detected. The Fe3O4/α-FeOOH ratio of the corrosion scales in P2 was higher those in P1 and P3, indicating P2 was in a relatively more active corrosion status than P1 and P3. The M/G ratio almost kept unchanged during the operation period. The formation of FeCO3 and CaCO3 verified the increase of alkalinity and calcium hardness inhibited the iron release. The bacterial communities were significantly affected by water quality. The total relative abundance of sulfur-oxidizing bacteria (SOB, e.g. Thiobacillus, Sulfurospirillum, Sulfurimonas and Alicyclobacillus), sulfate-reducing bacteria (SRB, e.g. Desulfitobacterium and Desulfurivibrio) and iron-oxidizing bacteria (IOB, e.g. Acidovorax, Ralstonia and Gallionella) increased significantly, while that of iron-reducing bacteria (IRB, e.g. Pseudomonas, Shewanella, Clostridium, Escherichia, Geothrix and Bacillus) almost remain unchanged. The BrO3− and Br-DBPs formation were enhanced at different degrees in the presence of CCPs, while the presence of HA significantly suppressed the BrO3− formation due to its strong competition for HOBr.The BrO3− formation was primarily promoted in the HOCl/Br−/CuO system, while the Br-DBPs formation was primarily promoted in the HOCl/Br−/Cu2O and HOCl/Br−/Cu2+ systems.The catalytic formation of BrO3− and Br-DBPs was highly dependent on pH. The degree of enhancement on the Br-DBPs formation became more apparent under an alkaline condition, while the BrO3− formation reached the maximum under a nearly neutral condition. The formation of Br-DBPs was considerably affected by the doses of Cu2O and Cu2+, while the BrO3− yield was significantly affected by the CuO dose. The increasing Br− concentration enhanced the catalytic formation of BrO3−, while the enhancement on the catalytic formation of Br-DBPs was not obviously observed. The characteristics of the real waters, such as inorganic irons and organic compositions, had an important impact on the formation of BrO3− and Br-DBPs in the presence of CCPs. The IPM degradation rate in the CuO/PMS system (CuPS) was much higher than that in the δ-MnO2/PMS system (MnPS). IPM was mainly degraded by sulfate radical (SO4•−) in the CuPS, while hydroxyl radical (HO•) also played an important role in the MnPS. The radical yield ratios were 0.89 and 0.69 mol/mol in the CuPS and MnPS, respectively. The IPM degradation rate increased with increasing PMS dose, and reached a maximum with a PCP dose of 1.0 and 1.5 g L–1 in the CuPS and MnPS, respectively. The highest degradation efficiency was achieved at pH 7.0. The water matrix (i.e., NOM, alkalinity and Cl−) inhibited IPM degradation to different degrees in the two systems. The majority of the iodine released from IPM was oxidized to IO3− and a small fraction of initial total organic iodine (TOI) was transformed to CHI3. The IPM degradation by PMS mainly proceeded through two pathways: 1) amide hydrolysis of side chain A, amino oxidation, and amide hydrolysis of side chains B and B' in sequence; and 2) deiodination reactions. The degradation rates of the three I-DBPs (i.e., CHI3, CHI2CONH2 and CI3COOH) under VUV/UV irradiation were higher than those under UV irradiation. The UV and VUV/UV were the most favorable for the degradation of CHI3, followed by CHI2CONH2 and then CI3COOH. The degradation of the three I-DBPs under VUV/UV irradiation was mainly attributed to the UV photodegradation. The degradation of the three I-DBPs proceeded via deiodination reaction step by step. The iodine released from the three I-DBPs to form I− under UV irradiation, and the formed I− was further oxidized to IO3− under VUV/UV irradiation. The degradation rates of the three I-DBPs increased with increasing pH under UV irradiation, while decreased with increasing pH under VUV/UV irradiation. The water matrix (i.e., NOM, HCO3− and Cl−) inhibited the degradation of the three I-DBPs to different degrees under UV and VUV/UV irradiation. This work specialized on the influence of water quality on the PCPs and bacterial community in DWDS, the effect of PCPs on the formation of DBPs and the removal of DBPs during secondary and terminal water supply, which was beneficial to control the formation of DBPs and the release of metal, to prevent the “secondary pollution” during water transportion, and to guarantee the safety of drinking water.
内容类型: 学位论文
URI标识: http://ir.rcees.ac.cn/handle/311016/38633
Appears in Collections:环境水质学国家重点实验室_学位论文

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