高分子铝盐优化混凝控制水中腐殖酸特性研究
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摘要
本研究针对给水源水中消毒副产物前驱物的去除这一热点,考察了高Al13/Al30含量聚合氯化铝和无机复合型聚硫氯化铝两类高分子铝盐混凝剂优化混凝去除水中主要消毒副产物前驱物—腐殖酸的特性,并对其作用机理进行探讨。
文章首先对消毒副产物的危害和控制技术、混凝和优化混凝应用基础以及高分子铝盐混凝剂的开发利用、形态表征、发展方向等进行了综述性研究。对混凝去除的目标物质—腐殖酸以及实验室配制的腐殖酸模拟水样的相关特性进行了表征,为水中腐殖酸的混凝去除研究打下基础。
在实验室制备了总铝浓度为0.2mol/L,碱化度(B=[OH-]／[Al3+])分别为1.2、1.8和2.4,分别以Al13和Al30为主要铝水解形态的聚合氯化铝十三(PAC-Al13)和聚合氯化铝三十(PAC-Al30)混凝剂。并通过在聚合铝盐的制备过程中引入一定量S042-离子,制备得到总铝浓度为0.2mol/L,碱化度为2.0,硫酸根投加比(S=[SO42-]／[Al3+])分别为0.00、0.02、0.06以及0.10的聚硫氯化铝(PACS)和高聚聚硫氯化铝(HPACS)昆凝剂,用于水中腐殖酸的混凝去除。
采用烧杯混凝沉淀实验方法,并以传统单分子混凝剂AlCl3做对照,从水样初始pH、混凝剂投量、共存阳离子和无机颗粒、电中和性能以及絮体形成能力等角度,分别考察了包含PAC-Al13、PAC-Al30、PACS以及HPACS在内的4个系列共14种高分子铝盐混凝剂去除水中腐殖酸的特性。实验结果表明,PAC-Al13、 PAC-Al30、PACS以及HPACS对腐殖酸的最佳去除效率分别达到97.6%、98.5%、99.4%和97.3%。水样初始pH、混凝剂投量对不同B值的PAC-Al13和PAC-Al30以及不同S值的PACS和HPACS有不同程度的影响；B值为2.4的PAC-Al13和PAC-Al30混凝性能优于其它碱化度的PAC-Al13和PAC-Al30混凝剂；S=0.06为PACS和HPACS混凝剂最佳的SO42-投加控制值；PAC-Al30(B=2.4)相比PAC-Al13(B=2.4)能在低投量下发挥更好的腐殖酸去除能力,且在大投量下不易出现混凝再稳现象；虽然PACS(S=0.06)对腐殖酸的去除效果最好,达到99.4%,但其获得最高腐殖酸去除率时所需的投量比HPACS(S=0.06)大,且HPACS(S=0.06)能在小投量以及偏碱性条件下获得更好的腐殖酸去除效果。在实际应用中应根据处理水质选择合适的混凝剂种类和投量。Ca2+和高岭土在混凝剂投量较小时分别通过压缩双电层和粘附架桥促进腐殖酸的混凝去除,而在混凝剂足量时作用不明显。除了水中腐殖酸的去除效果,对混凝出水残留铝浓度以及出水pH进行了测定,结果表明,高分子铝盐在多数情况下混凝出水残留铝浓度以及出水pH均达到居民生活饮用水卫生标准,相比之下单分子铝盐AlCl3的使用存在较多出水残留铝以及出水pH超标情况。
文章采用多种表征和鉴定手段,对制备的混凝剂进行了结晶形貌、电镜扫描(SEM)、X射线衍射(XRD)、傅里叶转换红外光谱(FTIR)、Al-Ferron逐时络合比色、激光散射粒径、密度以及吸湿性等物理化学特性分析,并结合其在混凝过程中的特性,对高分子铝盐优化混凝去除水中腐殖酸的作用机理进行了分析和探讨。研究发现,采用简单的浓缩结晶方法,可以从宏观角度观察到聚合氯化铝分枝形貌以及棱状结晶体图像,与文献中通过SEM、透射电镜(TEM)以及原子力显微镜(AFM)得到的显微图像相似；Al-Ferron逐时络合比色形态分析得到的以Al30等高聚合形态为主要成分的Alc有可能发挥出比中等聚合形态Alb更优越的混凝作用；混凝剂的激光散射粒径、密度、吸湿性等物理化学特性能在一定程度上影响或反映混凝剂的混凝效能。
本研究为新型高分子铝盐混凝剂的开发和应用打下基础,对于研制开发高性能的聚合铝盐混凝剂具有十分重要的理论和现实意义。此外,实验对最佳混凝条件的探索和各种影响因素的分析,将为以腐殖酸为代表的消毒副产物前驱物的控制技术提供经济可行的优化混凝参考方案。
High Al13/Al30contend polyaluminum chlorides and inorganic composite polyaluminum with sulfate were developed, and the the coagulation behavior of them were investigased for humic acid (one typical disinfection by-products (DBPs) precursor) removal. The mechanisms of coagulation were investigated simultaneously.
Firstly, hazards and control technologies of DBPs, application of coagulation and optimized coagulation, and development, application and characterization of polymeric aluminum coagulants were reviewed in this article. Then, the commercial humic acids (HA) were analyzed by modern analytical methods, and the properties of simulated raw water with the commercial HA were studied.
Polyaluminum chlorides with a high Al13content (PAC-Al13) and with a high Al30content (PAC-Al30) were prepared in laboratory for HA removal. The basicity (B=[OH-]/[A13+]) of PAC-Al13and PAC-Al30was controlled to be1.2.1.8, and2.4respectively. Poly-Aluminum Chloride Sulfate (PACS) and High-Poly-Aluminum Chloride Sulfate (HPACS) coagulants were prepared by adding SO42-in preparation process of polyaluminum chlorides. The sulfate addition ratio (S=[SO42-]/[A13+]) was0.00,0.02,0.06and0.10respectively.
Compared with AICl3, coagulation behaviors of PAC-Al13、PAC-Al30、PACS and HPACS were investigated by jar tests, and the influence of initial pH, coagulation dosage, coexisting cations and inorganic particles, the charge neutralization performance and the floc formation capacity were considered. The results showed that the best HA removal efficiency of PAC-Al13、PAC-Al30、PACS and HPACS were97.6%、98.5%、99.4%and97.3%, respectively. Initial pH and coagulants dosage showed different effects on the coagulation of PAC-Al13and PAC-Al30with different B values, and PACS and HPACS with different S values. Generally, PAC-Al13and PAC-Al30with the B value of2.4showed more excellent coagulation effect than the other PAC coagulants, and S=0.06was the best choice for PACS and HPACS preparation. PAC-Al30(B=2.4) not only performed a more effective HA removal at low coagulant dosage but also exhibited less re-stabilization at a high dosage, compared with PAC-Al13(B=2.4) and AlCl3. Although PACS (S=0.06) achieved the highest HA removal efficiency of99.4%. higher coagulant dosage of PACS (S=0.06) was needed to get the best HA removal than that of HPACS (S=0.06). HPACS (S=0.06) performed a more effective HA removal at the low coagulant dosage and in a basic medium, compared with PACS (S=0.06). The appropriate type and dosage of coagulants should be optimized based on the source water quality in practice. When the coagulant dosage was low, the exsiting of Ca2+and kaolin promoted HA removal through double-layer compression and bridging adsorption, but these effects became insignificant when the coagulant dosage was sufficient. Besides HA removal, the residual Al concentration and pH of the treated water were also investigated. The results indicated that residual Al concentration and pH met the requirement of drinking water quality for polymeric aluminum coagulants application under most conditions, while AICI3might be not suitable for source water treatment from this consideration.
Crystal morphology, scanning electron microscopy (SEM), X-ray diffraction (XRD), fourier transform infrared spectroscopy (FTIR), Al-Ferron timed complexation colorimetric and some other physical and chemical properties like laser scattering particle size, dencity and hygroscopic etc. of prepared coagulants were studied, and the coagulation mechanisms of HA removal were discussed combining with the coagulate characteristics. The branching morphology and prismatic crystals of polymeric aluminum, which usually were observed by SEM or AMF, were found with the simple crystallization. The Alc detected by Al-Ferron timed complexation colorimetric might be more effective for HA coagulation than the Alb-The laser scattering particle size, dencity and hygroscopic of coagulants also reflected and affected the coagulation performance to some extent.
This study provides a foundation for development and application of new polymeric aluminum coagulants, showing an important theoretical and practical significance for development of high-effective coagulants. The optimal coagulation conditions and the analysis of influence factors would provide a cost-effective apporch for HA removal by optimized coagulation.
文章首先对消毒副产物的危害和控制技术、混凝和优化混凝应用基础以及高分子铝盐混凝剂的开发利用、形态表征、发展方向等进行了综述性研究。对混凝去除的目标物质—腐殖酸以及实验室配制的腐殖酸模拟水样的相关特性进行了表征,为水中腐殖酸的混凝去除研究打下基础。
在实验室制备了总铝浓度为0.2mol/L,碱化度(B=[OH-]／[Al3+])分别为1.2、1.8和2.4,分别以Al13和Al30为主要铝水解形态的聚合氯化铝十三(PAC-Al13)和聚合氯化铝三十(PAC-Al30)混凝剂。并通过在聚合铝盐的制备过程中引入一定量S042-离子,制备得到总铝浓度为0.2mol/L,碱化度为2.0,硫酸根投加比(S=[SO42-]／[Al3+])分别为0.00、0.02、0.06以及0.10的聚硫氯化铝(PACS)和高聚聚硫氯化铝(HPACS)昆凝剂,用于水中腐殖酸的混凝去除。
采用烧杯混凝沉淀实验方法,并以传统单分子混凝剂AlCl3做对照,从水样初始pH、混凝剂投量、共存阳离子和无机颗粒、电中和性能以及絮体形成能力等角度,分别考察了包含PAC-Al13、PAC-Al30、PACS以及HPACS在内的4个系列共14种高分子铝盐混凝剂去除水中腐殖酸的特性。实验结果表明,PAC-Al13、 PAC-Al30、PACS以及HPACS对腐殖酸的最佳去除效率分别达到97.6%、98.5%、99.4%和97.3%。水样初始pH、混凝剂投量对不同B值的PAC-Al13和PAC-Al30以及不同S值的PACS和HPACS有不同程度的影响；B值为2.4的PAC-Al13和PAC-Al30混凝性能优于其它碱化度的PAC-Al13和PAC-Al30混凝剂；S=0.06为PACS和HPACS混凝剂最佳的SO42-投加控制值；PAC-Al30(B=2.4)相比PAC-Al13(B=2.4)能在低投量下发挥更好的腐殖酸去除能力,且在大投量下不易出现混凝再稳现象；虽然PACS(S=0.06)对腐殖酸的去除效果最好,达到99.4%,但其获得最高腐殖酸去除率时所需的投量比HPACS(S=0.06)大,且HPACS(S=0.06)能在小投量以及偏碱性条件下获得更好的腐殖酸去除效果。在实际应用中应根据处理水质选择合适的混凝剂种类和投量。Ca2+和高岭土在混凝剂投量较小时分别通过压缩双电层和粘附架桥促进腐殖酸的混凝去除,而在混凝剂足量时作用不明显。除了水中腐殖酸的去除效果,对混凝出水残留铝浓度以及出水pH进行了测定,结果表明,高分子铝盐在多数情况下混凝出水残留铝浓度以及出水pH均达到居民生活饮用水卫生标准,相比之下单分子铝盐AlCl3的使用存在较多出水残留铝以及出水pH超标情况。
文章采用多种表征和鉴定手段,对制备的混凝剂进行了结晶形貌、电镜扫描(SEM)、X射线衍射(XRD)、傅里叶转换红外光谱(FTIR)、Al-Ferron逐时络合比色、激光散射粒径、密度以及吸湿性等物理化学特性分析,并结合其在混凝过程中的特性,对高分子铝盐优化混凝去除水中腐殖酸的作用机理进行了分析和探讨。研究发现,采用简单的浓缩结晶方法,可以从宏观角度观察到聚合氯化铝分枝形貌以及棱状结晶体图像,与文献中通过SEM、透射电镜(TEM)以及原子力显微镜(AFM)得到的显微图像相似；Al-Ferron逐时络合比色形态分析得到的以Al30等高聚合形态为主要成分的Alc有可能发挥出比中等聚合形态Alb更优越的混凝作用；混凝剂的激光散射粒径、密度、吸湿性等物理化学特性能在一定程度上影响或反映混凝剂的混凝效能。
本研究为新型高分子铝盐混凝剂的开发和应用打下基础,对于研制开发高性能的聚合铝盐混凝剂具有十分重要的理论和现实意义。此外,实验对最佳混凝条件的探索和各种影响因素的分析,将为以腐殖酸为代表的消毒副产物前驱物的控制技术提供经济可行的优化混凝参考方案。
High Al13/Al30contend polyaluminum chlorides and inorganic composite polyaluminum with sulfate were developed, and the the coagulation behavior of them were investigased for humic acid (one typical disinfection by-products (DBPs) precursor) removal. The mechanisms of coagulation were investigated simultaneously.
Firstly, hazards and control technologies of DBPs, application of coagulation and optimized coagulation, and development, application and characterization of polymeric aluminum coagulants were reviewed in this article. Then, the commercial humic acids (HA) were analyzed by modern analytical methods, and the properties of simulated raw water with the commercial HA were studied.
Polyaluminum chlorides with a high Al13content (PAC-Al13) and with a high Al30content (PAC-Al30) were prepared in laboratory for HA removal. The basicity (B=[OH-]/[A13+]) of PAC-Al13and PAC-Al30was controlled to be1.2.1.8, and2.4respectively. Poly-Aluminum Chloride Sulfate (PACS) and High-Poly-Aluminum Chloride Sulfate (HPACS) coagulants were prepared by adding SO42-in preparation process of polyaluminum chlorides. The sulfate addition ratio (S=[SO42-]/[A13+]) was0.00,0.02,0.06and0.10respectively.
Compared with AICl3, coagulation behaviors of PAC-Al13、PAC-Al30、PACS and HPACS were investigated by jar tests, and the influence of initial pH, coagulation dosage, coexisting cations and inorganic particles, the charge neutralization performance and the floc formation capacity were considered. The results showed that the best HA removal efficiency of PAC-Al13、PAC-Al30、PACS and HPACS were97.6%、98.5%、99.4%and97.3%, respectively. Initial pH and coagulants dosage showed different effects on the coagulation of PAC-Al13and PAC-Al30with different B values, and PACS and HPACS with different S values. Generally, PAC-Al13and PAC-Al30with the B value of2.4showed more excellent coagulation effect than the other PAC coagulants, and S=0.06was the best choice for PACS and HPACS preparation. PAC-Al30(B=2.4) not only performed a more effective HA removal at low coagulant dosage but also exhibited less re-stabilization at a high dosage, compared with PAC-Al13(B=2.4) and AlCl3. Although PACS (S=0.06) achieved the highest HA removal efficiency of99.4%. higher coagulant dosage of PACS (S=0.06) was needed to get the best HA removal than that of HPACS (S=0.06). HPACS (S=0.06) performed a more effective HA removal at the low coagulant dosage and in a basic medium, compared with PACS (S=0.06). The appropriate type and dosage of coagulants should be optimized based on the source water quality in practice. When the coagulant dosage was low, the exsiting of Ca2+and kaolin promoted HA removal through double-layer compression and bridging adsorption, but these effects became insignificant when the coagulant dosage was sufficient. Besides HA removal, the residual Al concentration and pH of the treated water were also investigated. The results indicated that residual Al concentration and pH met the requirement of drinking water quality for polymeric aluminum coagulants application under most conditions, while AICI3might be not suitable for source water treatment from this consideration.
Crystal morphology, scanning electron microscopy (SEM), X-ray diffraction (XRD), fourier transform infrared spectroscopy (FTIR), Al-Ferron timed complexation colorimetric and some other physical and chemical properties like laser scattering particle size, dencity and hygroscopic etc. of prepared coagulants were studied, and the coagulation mechanisms of HA removal were discussed combining with the coagulate characteristics. The branching morphology and prismatic crystals of polymeric aluminum, which usually were observed by SEM or AMF, were found with the simple crystallization. The Alc detected by Al-Ferron timed complexation colorimetric might be more effective for HA coagulation than the Alb-The laser scattering particle size, dencity and hygroscopic of coagulants also reflected and affected the coagulation performance to some extent.
This study provides a foundation for development and application of new polymeric aluminum coagulants, showing an important theoretical and practical significance for development of high-effective coagulants. The optimal coagulation conditions and the analysis of influence factors would provide a cost-effective apporch for HA removal by optimized coagulation.
引文
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