中文题名: | 水铁矿-超滤膜组合工艺对有机物和As(III)的协同去除机制及对膜污染的控制研究 |
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保密级别: | 公开 |
论文语种: | 中文 |
学科代码: | 083002 |
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学生类型: | 硕士 |
学位: | 工学硕士 |
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学位年度: | 2018 |
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研究方向: | 饮用水处理 |
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提交日期: | 2018-06-19 |
答辩日期: | 2018-06-19 |
外文题名: | SYNERGETIC REMOVAL OF ORGANIC MATTER AND As(III) AND CONTROL OF MEMBRANE FOULING BY A HYBRID FERRIHYDRITE-ULTRAFILTRATION PROCESS |
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中文摘要: |
超滤(Ultrafiltration, UF)膜技术广泛应用于饮用水处理领域,但是UF膜孔相对较大,对溶解性有机物(Dissolved organic matter,DOM)和无机离子的去除率较低,对消毒副产物(Disinfection by-products,DBPs)的控制效果较差;膜污染问题限制了膜技术的推广应用。因此,本文基于水铁矿(Ferrihydrite,FH)对As及DOM的高效去除能力,构建FH-UF膜组合工艺,控制水体中消毒副产物生成势(Disinfection by-product formation potentials,DBPFPs),并减少膜污染负荷。揭示了FH预吸附-膜组合工艺在控制消毒副产物以及膜污染方面的应用潜能,为保障饮用水安全和吸附-膜组合工艺的应用提供了科学基础与技术支持。
选择腐殖酸(Humic acid,HA)、海藻酸钠(Sodium alginate,SA)和牛血清蛋白(Bovine serum albumin,BSA)三种模型污染物代表不同组分的DOM,通过吸附平衡与动力学实验,探究有机物在FH表面的作用机制及吸附特征。实验结果表明,FH和PAC对三种有机组分的吸附符合准二阶动力学与Freundlich模型。采用排阻色谱法、三维荧光光谱等化学表征手段,对照吸附与膜分离单元对不同有机组分的协同作用机制,同时将宏观上跨膜压差的变化与微观形貌分析、膜阻变化与膜污染组分分析相结合,探究组合工艺中吸附剂FH对滤饼层结构及膜污染的影响,为膜污染控制提供理论依据。实验结果表明,FH-UF膜组合工艺对三种有机物组分的去除率都高于PAC-UF膜组合工艺。FH有效吸附了大分子有机物,减少了大分子有机物在UF膜表面的富集,形成了疏松的FH滤饼层,FH-UF膜组合工艺显著地减轻了三种有机组分引起的膜污染。PAC优先吸附小分子有机物,显著降低了BSA分子引起的膜污染;PAC难以吸附大分子有机物,并形成了致密的滤饼层,但对HA和SA分子引起的膜污染影响较小。
天然有机质(Suwannee River natural organic matter,SRNOM)与As的配水研究表明,FH和PAC对As(III)的吸附符合准二阶动力学与Langmuir模型,对SRNOM的吸附符合准二阶动力学与Freundlich模型。FH和PAC对As(III)的吸附能力均在中性条件下最强,对SRNOM的吸附能力都是随着pH的升高而降低。通过考察组合工艺对As(III)和SRNOM的去除效果以及对UF膜污染的控制效果,揭示了不同组成对DBPFPs以及致癌因子的贡献及影响。结果表明,基于FH对As(III)和DOM的强吸附能力,FH-UF膜组合工艺对As(III)和DOM的去除率分别达到了99.4%与81.8%,均高于PAC-UF膜组合工艺。FH-UF膜组合工艺显著地减轻了膜污染,PAC-UF膜组合工艺对膜污染影响较小。由于FH对溶液中芳香类有机物的去除率较高,FH-UF膜组合工艺显著降低了DBPFPs,且FH有效吸附了溶液中的可溶性微生物副产物(Soluble microbial by-product,SMP)类有机物,这类有机物是溴代消毒副产物(Brominated disinfection by-products,Br-DBPs)的主要前体物。PAC对该类有机物的去除能力较弱,导致PAC-UF膜组合工艺对Br-DBPs的控制效果较差。因此,FH-UF膜组合工艺有效地去除了DBPs前体物,并显著地降低了As(III)和DBPs的致癌风险,As(III)浓度与DBPs的产生量均低于世界卫生组织(WHO)饮用水标准。
选取北京市天然地表水,考察了FH和PAC对天然地表水中有机物的吸附能力以及FH-UF膜组合工艺对天然地表水中有机物的去除效果以及对UF膜污染的控制情况。实验结果表明:FH对天然地表水中有机物的吸附速率与吸附能力均高于PAC,且FH对天然地表水中腐殖质类、芳香蛋白类与可溶性微生物副产物类有机物都具有较强的吸附能力。FH-UF膜组合工艺对天然水体中有机物的去除率达到了74.6%,芳香类有机物的去除率高达93.5%,均高于PAC-UF膜组合工艺。此外,FH-UF膜组合工艺降低了62.4%的UF膜阻,有效缓解了膜污染。
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外文摘要: |
Ultrafiltration (UF) membrane is a promising approach used in drinking water treatment processes. However, a UF membrane with a relatively large pore size is not effective in removing dissolved organic matter (DOM) and inorganic ions. Thus, it is hard for UF to control disinfection by-products (DBPs). Besides, membrane fouling limits the more widespread application of UF membranes. Based on the large As and DOM adsorption capacity of ferrihydrite (FH), the hybrid FH-UF membrane process was constructed to control disinfection by-product formation potentials (DBPFPs) in water and to reduce the membrane fouling load.
Three model foulants, namely, humic acid (HA), sodium alginate (SA) and bovine serum albumin (BSA), were applied in feed water to simulate different DOM fractions. The adsorption mechanism and adsorption characteristics of three DOM fractions on the surface of FH were studied by adsorption equilibrium and kinetic experiments. The experimental results showed that the pseudo-second-order model and the Freundlich model fit well with the adsorption of FH and PAC on the three DOM components. The synergistic mechanism of adsorption and membrane separation on different organic components was investigated through size exclusion chromatography and fluorescence excitation-emission matrix. The variation of transmembrane pressure (TMP) and membrane resisitance and the analysis of microscopic morphology and membrane foulant components were combined to explore the influence of FH on the structure of cake layer and membrane fouling and provide theoretical basis for membrane fouling control. The experimental results showed that the removal efficiency of the three organic components by hybrid FH-UF process is higher than that of hybrid PAC-UF process. FH effectively adsorbed high molecular weight (MW) DOM molecules, and reduced the enrichment of macromolecule DOM on the surface of UF membrane and formed a loose FH cake layer. Hybrid FH-UF process significantly alleviated the membrane fouling caused by three DOM components. PAC preferentially adsorbed low-MW DOM molecules, and significantly reduced the membrane fouling caused by BSA molecules. PAC exhibited a weak adsorption capacity on high-MW HA and SA molecules and the PAC cake layer was dense. Thus, hybrid PAC-UF process didn’t alleviate the membrane fouling caused by HA and SA molecules.
The study of synthetic water containing Suwannee River natural organic matter (SRNOM) and As(III) showed that the pseudo-second-order model and the Langmuir model fit well with the adsorption of FH and PAC on As(III) while the pseudo-second-order model and the Freundlich model fit well with the adsorption of FH and PAC on SRNOM. The As(III) adsorption ability of FH and PAC was the strongest under neutral condition and the SRNOM adsorption ability of two adsorbents decreased with the increase of pH in the solution. The effects of the hybrid process on the removal of As(III) and SRNOM and on the control of UF membrane fouling were investigated. The contribution and effect of different components to DBPFPs and cancer risks (CRs) were revealed. The results showed that the removal rates of As(III) and DOM by hybrid FH-UF process were 99.4% and 81.8%, respectively, which were higher than those by hybrid PAC-UF process. The main reason for this result was mainly due to the large As(III) and DOM adsorption ability of FH. Hybrid FH-UF process mitigated membrane fouling significantly whereas hybrid PAC-UF process didn’t alleviate membrane fouling. Due to the large aromatic DOM adsorption ability of FH, hybrid FH-UF process reduced DBP formation potential substantially. In addition, FH exhibited a large adsorption capacity for soluble microbial by-product (SMP)-like matter, which was the main brominated DBP (Br-DBP) precursor. Thus, hybrid FH-UF process removed DBP precursors efficiently and declined the CRs from As(III) and DBPs. After hybrid FH-UF process treated, the concentrations of As(III) and every DBP were lower than the World Health Organization (WHO) guideline values for drinking water.
The water from Beijing Jingmi aqueduct as natural surface water (NSW).The adsorption capacity of FH and PAC for DOM in NSW, the removal of DOM from NSW and the control of UF membrane fouling by hybrid FH-UF process were investigated. The results showed that the adsorption rate and adsorption capacity of DOM in NSW by FH was stronger than that by PAC and FH showed a large adsorption capacity for all kinds of DOM in NSW. The removal rates of DOC and UV254 in NSW by hybrid FH-UF process were 74.6% and 93.5%, respectively, which were higher than those by hybrid PAC-UF process. In addition, hybrid FH-UF process reduced 62.4% of the resisitance of UF membrane and mitigated membrane fouling efficiently.
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参考文献总数: | 141 |
作者简介: | 攻读硕士期间取得的学术成果 期刊论文 Sen Zhang, Yu Yang*, Satoshi Takizawa, Li-an Hou. Removal of DOM and control of membrane fouling by a hybrid a ferrihydrite-ultrafiltration membrane system [J]. Science of the Total Environment, 631–632 (2018) 560–569. 会议论文 杨禹, 张森. 水铁矿-超滤膜组合工艺对消毒副产物和膜污染的控制[C]. 第九届全国环境化学大会, 杭州, 2017. 专利 杨禹, 张森, 侯立安. 去除三价砷与消毒副产物前体物的水铁矿-UF膜组合工艺. CN 201810281661. |
馆藏号: | 硕083002/18025 |
开放日期: | 2019-07-09 |