活性炭—超滤复合工艺去除水中典型PPCPs的效能与机理
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摘要
饮用水中药品与个人护理品（PPCPs）正受到世界范围的广泛关注，而国内尚未见报道。本文采用高效液相色谱串联质谱法，调查了珠三角地区典型城市饮用水系统中39种PPCPs的分布、归宿和影响。结合气候和水源水质特征，提出了活性炭-超滤复合工艺，研究了典型PPCPs在复合工艺中的行为与机理。评价了复合工艺对典型PPCPs与其他污染物的去除效能，研究成果应用于规模为4万m~3·d~(-1)的示范工程。
水源中16种PPCPs的检出浓度为ND~27ng·L~(-1)。出厂水中12种PPCPs的检出浓度为ND~5ng·L~(-1)，深度处理工艺对大多数PPCPs的去除效果优于常规处理工艺。管网水和龙头水分别有15种和17种PPCPs检出，浓度均为1ng·L~(-1)左右。典型PPCPs混合物对斑马鱼胚胎发育的影响浓度为ng·L~(-1)水平，与水源中PPCPs的检出浓度相当，有潜在的生态和健康风险。
活性炭去除PPCPs的机理包括活性炭吸附与有机物竞争吸附。活性炭对典型PPCPs的吸附符合指数衰减模型，其动力学吸附系数（Kd）为0.0067~0.0133min~(-1)。溶液pH降低，Kd会不断增加；腐殖酸存在时，Kd会降低20~47%。典型PPCPs吸附行为受其物化性质与活性炭的结构特征等影响。在典型PPCPs胁迫下，微生物种群结构会明显变化，有机会致病菌出现。
超滤去除PPCPs的机理包括超滤膜吸附以及有机物或颗粒物协同吸附。溶液pH值降低会提高超滤膜对典型PPCPs的去除率。腐殖酸和颗粒物能改善超滤膜对典型PPCPs的去除效果，其去除率随腐殖酸和颗粒物浓度的升高而增加，而受颗粒物粒径的影响较小。有机碳分配系数（Koc）对典型PPCPs吸附行为有重要影响，而酸度系数（pKa）的影响与否则与溶液pH等有关。
活性炭-超滤复合工艺对典型PPCPs的去除率为30~100%，其中，活性炭工艺占75~90%。在活性炭工艺中，活性炭吸附和微生物降解分别占94%和6％。典型PPCPs的去除效果受进水PPCPs浓度、滤速、pH、有机物、炭层高、活性炭性能、超滤膜特性和臭氧等影响。
活性炭-超滤复合工艺对浊度、颗粒数、有机物和微生物等去除效果较好。炭层厚和滤速对活性炭工艺的运行有重要影响。进水水质、运行参数、超滤膜类型和膜性能变化等会影响超滤运行。超滤膜污染由有机物、金属和微生物等综合所致。
Pharmaceuticals and personal care products (PPCPs) in drinking water havebeen receiving extensive attention all over the world. However, no paper hasbeen reported about them in China. In this study, occurrence, fate and effect of39PPCPs in drinking water were investigated in southern China by highperformance liquid chromatography and tandem mass spectrometry(HPLC/MS/MS). Hybrid processes with granular activated carbon (GAC) andultrafiltration (UF) was developed based on the characteristics of climate andsource water quality. Performance of the hybrid processes in the removal oftypical PPCPs and other pollutants was evaluated. Behaviors and mechanisms oftypical PPCPs removal by the hybrid processes were investigated. A full-scalewater treatment plant was established on basis of the experimental results, withthe capacity of400000m~3·d~(-1).
The concentrations of sixteen PPCPs detected in source water were ND~27ng·L~(-1). Twelve PPCPs were detected in treated water, with concentration ofND~5ng·L~(-1). Advanced treatment processes were more efficient in the removalof most PPCPs than conventional treatment processes. Fifteen and seventeenPPCPs were detected in pipeline and tap water, respectively, with concentrationof1ng·L~(-1). Typical PPCPs mixture had an influence on zebrafish embryodevelopment at the level of ng·L~(-1). Some potential ecological and health riskscaused by PPCPs existed for water sources in southern China.
Removal mechanisms of typical PPCPs by GAC included GAC adsorptionand organic competition. Adsorption kinetics of typical PPCPs to GAC fittedexponential decay model. Adsorption coefficients (Kd) of the PPCPs were0.0067~0.0133min~(-1). Kdincreased with decreasing pH values, but decreased by20~47%in humic acid (HA) solution. Adsorption behaviors of the PPCPs wereinfluenced by their physiochemical properties and GAC structure characteristics.Population structure of microorganisms changed obviously under the typicalPPCPs stress, with a lot of opportunity bacteria detected.
Removal mechanisms of typical PPCPs by UF included UF membraneadsorption and cooperative adsorption by HA or particles. The PPCPs removals by UF increased with decreasing pH values. HA and particles improved theremovals of the PPCPs by UF. The removals increased with increasingconcentration of HA and particles, but changed little with particle size. Organiccarbon partition coefficient (Koc) had an important influence on adsorptionbehaviors of typical PPCPs. The influence of acidity coefficient (pKa) wasrelated to the solution pH.
The hybrid processes removed typical PPCPs by30~100%, with75~90%ofthem removed by GAC. GAC adsorption and biodegradation accounted for94%and6%, respectively during GAC treatment. The removal efficiencies of thePPCPs were affected by PPCPs concentration in the influent, filtration velocity,pH, organic matter, GAC media height, GAC characteristic, membraneproperties and ozonation.
The hybrid processes removed turbidity, particles, organic matter andmicroorganisms effectively. The height of GAC media layer and filtrationvelocity of GAC process had an important effect on the performance of GACprocess. UF performance was affected by water quality, operation parameters,membrane types and the changes of membrane properties. UF membrane foulingwas caused by organic matter, metal ions and microorganisms.
水源中16种PPCPs的检出浓度为ND~27ng·L~(-1)。出厂水中12种PPCPs的检出浓度为ND~5ng·L~(-1)，深度处理工艺对大多数PPCPs的去除效果优于常规处理工艺。管网水和龙头水分别有15种和17种PPCPs检出，浓度均为1ng·L~(-1)左右。典型PPCPs混合物对斑马鱼胚胎发育的影响浓度为ng·L~(-1)水平，与水源中PPCPs的检出浓度相当，有潜在的生态和健康风险。
活性炭去除PPCPs的机理包括活性炭吸附与有机物竞争吸附。活性炭对典型PPCPs的吸附符合指数衰减模型，其动力学吸附系数（Kd）为0.0067~0.0133min~(-1)。溶液pH降低，Kd会不断增加；腐殖酸存在时，Kd会降低20~47%。典型PPCPs吸附行为受其物化性质与活性炭的结构特征等影响。在典型PPCPs胁迫下，微生物种群结构会明显变化，有机会致病菌出现。
超滤去除PPCPs的机理包括超滤膜吸附以及有机物或颗粒物协同吸附。溶液pH值降低会提高超滤膜对典型PPCPs的去除率。腐殖酸和颗粒物能改善超滤膜对典型PPCPs的去除效果，其去除率随腐殖酸和颗粒物浓度的升高而增加，而受颗粒物粒径的影响较小。有机碳分配系数（Koc）对典型PPCPs吸附行为有重要影响，而酸度系数（pKa）的影响与否则与溶液pH等有关。
活性炭-超滤复合工艺对典型PPCPs的去除率为30~100%，其中，活性炭工艺占75~90%。在活性炭工艺中，活性炭吸附和微生物降解分别占94%和6％。典型PPCPs的去除效果受进水PPCPs浓度、滤速、pH、有机物、炭层高、活性炭性能、超滤膜特性和臭氧等影响。
活性炭-超滤复合工艺对浊度、颗粒数、有机物和微生物等去除效果较好。炭层厚和滤速对活性炭工艺的运行有重要影响。进水水质、运行参数、超滤膜类型和膜性能变化等会影响超滤运行。超滤膜污染由有机物、金属和微生物等综合所致。
Pharmaceuticals and personal care products (PPCPs) in drinking water havebeen receiving extensive attention all over the world. However, no paper hasbeen reported about them in China. In this study, occurrence, fate and effect of39PPCPs in drinking water were investigated in southern China by highperformance liquid chromatography and tandem mass spectrometry(HPLC/MS/MS). Hybrid processes with granular activated carbon (GAC) andultrafiltration (UF) was developed based on the characteristics of climate andsource water quality. Performance of the hybrid processes in the removal oftypical PPCPs and other pollutants was evaluated. Behaviors and mechanisms oftypical PPCPs removal by the hybrid processes were investigated. A full-scalewater treatment plant was established on basis of the experimental results, withthe capacity of400000m~3·d~(-1).
The concentrations of sixteen PPCPs detected in source water were ND~27ng·L~(-1). Twelve PPCPs were detected in treated water, with concentration ofND~5ng·L~(-1). Advanced treatment processes were more efficient in the removalof most PPCPs than conventional treatment processes. Fifteen and seventeenPPCPs were detected in pipeline and tap water, respectively, with concentrationof1ng·L~(-1). Typical PPCPs mixture had an influence on zebrafish embryodevelopment at the level of ng·L~(-1). Some potential ecological and health riskscaused by PPCPs existed for water sources in southern China.
Removal mechanisms of typical PPCPs by GAC included GAC adsorptionand organic competition. Adsorption kinetics of typical PPCPs to GAC fittedexponential decay model. Adsorption coefficients (Kd) of the PPCPs were0.0067~0.0133min~(-1). Kdincreased with decreasing pH values, but decreased by20~47%in humic acid (HA) solution. Adsorption behaviors of the PPCPs wereinfluenced by their physiochemical properties and GAC structure characteristics.Population structure of microorganisms changed obviously under the typicalPPCPs stress, with a lot of opportunity bacteria detected.
Removal mechanisms of typical PPCPs by UF included UF membraneadsorption and cooperative adsorption by HA or particles. The PPCPs removals by UF increased with decreasing pH values. HA and particles improved theremovals of the PPCPs by UF. The removals increased with increasingconcentration of HA and particles, but changed little with particle size. Organiccarbon partition coefficient (Koc) had an important influence on adsorptionbehaviors of typical PPCPs. The influence of acidity coefficient (pKa) wasrelated to the solution pH.
The hybrid processes removed typical PPCPs by30~100%, with75~90%ofthem removed by GAC. GAC adsorption and biodegradation accounted for94%and6%, respectively during GAC treatment. The removal efficiencies of thePPCPs were affected by PPCPs concentration in the influent, filtration velocity,pH, organic matter, GAC media height, GAC characteristic, membraneproperties and ozonation.
The hybrid processes removed turbidity, particles, organic matter andmicroorganisms effectively. The height of GAC media layer and filtrationvelocity of GAC process had an important effect on the performance of GACprocess. UF performance was affected by water quality, operation parameters,membrane types and the changes of membrane properties. UF membrane foulingwas caused by organic matter, metal ions and microorganisms.
引文
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