铝盐混凝剂在给水处理中残留铝含量、组分及影响机制研究
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摘要
本论文在综述国内外大量文献的基础上,首先建立并确定了净化水中不同组分残留铝的分离及测定方法,然后针对腐植酸-高岭土模拟地表水和不同季节引黄水库水的特点,对比研究了混凝剂种类、混凝剂合成条件、混凝剂投加量、水体初始pH及水力条件对混凝效果、残留铝含量、残留铝组分及余铝率的影响；从混凝效果和不同组分残留铝含量分别确定了各铝盐混凝剂处理不同地表水的最佳投加量以及最佳处理pH,并明确了各铝盐混凝剂在不同季节引黄水库水处理中的最佳作用水力条件；同时分析了影响残留铝含量的主要因素,探讨了混凝效果(絮体特性操作参数)与各组分残留铝浓度之间的关系。主要结论如下：
1.在腐植酸-高岭土模拟地表水混凝处理中,氯化铝、硫酸铝和聚合氯化铝(PAC)在不同投加量下的浊度和UV254去除率最高可达90%左右；PAC投加量较高时混凝效果较好,其混凝出水巾残留总铝量(约为0.9mg/L)和余铝率(-3.0%)均是三种混凝剂巾最低的,且PAC能够有效降低出水巾毒性较大的溶解性铝的含量(约为0.6mg／L)；在pH为6.0-7.0之间,氯化铝、硫酸铝和PAC的浊度去除率分别可达到94%,91.5%和90.5%,UV254去除率可分别达到87%,88.5%和82%；不同pH下PAC混凝出水中残留铝含量及余铝率最低；三种混凝剂在投加量范围为10-12mg／L下处理腐植酸-高岭土模拟地表水时可以取得最佳的混凝去除效果和最低的残留铝含量；但它们取得最佳混凝效果和最低残留铝含量的pH范围分别为6.0-7.0和7.0-8.0；三种混凝剂净化后水中残留铝均大部分以溶解性总铝的形式存在(约60%-80%),溶解性有机铝在总溶解性铝巾所占比例较大,溶解性单体铝组分基本均为溶解性无机单体铝。
2.PAC更适于春秋季节引黄水库水混凝处理,不同投加量和pH下具有比传统氯化铝混凝去除率更高、电中和能力更强、残留铝含量更低、混凝剂本身余铝率更低和对水体pH改变的适应性更强的优点；氯化铝和PAC的电中和能力在酸性条件下更强,两种混凝剂混凝出水中大部分是亲水性有机物,增加投加量以及中性和偏碱性条件更利于疏水性有机物的去除；不同条件下PAC中的铝不易残留,余铝率均明显低于氯化铝的余铝率,但其混凝出水中溶解性有机结合铝含量较高；PAC在春秋季节引黄水库水处理中,取得较好混凝效果的碱化度(B)为2.0、投加量范围为12-15mg/L、初始水体pH为6.0左右；净化后水中残留铝均大部分以溶解性总铝的形式存在,且溶解性有机铝在总溶解性铝中所占比例较大,溶解性单体铝主要以溶解性无机单体铝为主；各组分残留铝浓度及混凝剂余铝率均在投加量为12～15mg/L、pH为7.0-8.5下较低,可有效控制混凝出水中的残留铝含量；此外,B值为2.0的PAC在春季水库水处理巾余铝率较低。
3.在冬季低温低浊引黄水库水处理中,聚硅氯化铝(PASiC)以吸附架桥和卷扫絮凝为主，B值为2.0、硅铝摩尔比为0.05时PASiC具有更好的混凝效果和更低的残留铝含量；不论B值和硅铝摩尔比如何变化,PASiC均在投加量范围为12-15mg/L、初始pH为6.0-7.0时对引黄水库水中的浊度和有机物具有良好的去除效果,而在投加量为10～15mg/L、初始pH为7.0-8.5下PASiC混凝后水巾含有较低浓度的残留铝；PASiC更适宜于去除水库水巾疏水性和具有芳香族特性的大分子有机物;PASiC在冬季低温低浊引黄水库水处理中,混凝出水巾残留铝中大部分是总溶解性铝,在总溶解性铝中溶解性单体铝的成分最大,溶解性单体铝主要以溶解性无机单体铝为主;同使用PAC处理春秋季引黄水库水相比,使用PASiC(?)昆凝处理冬季低温低浊引黄水库水时混凝剂的最佳投加量较高
4.在夏季高藻引黄水库水处理中,向PAC中引入聚二甲基二烯丙基氯化铵(PDMDAAC)后制备出的聚合氯化铝-聚二甲基二烯丙基氯化铵(PAC-PDMDAAC)复合混凝剂的混凝特性受无机有机组分质量比(MR值)及B值的影响,B值为2.0、MR值为4：1时复合混凝剂的混凝效果较好；PAC-PDMDAAC处理夏季高藻引黄水库水的最佳投加量为6mg/L,最佳水体pH为6.0左右；B值为2.0、MR值为4：1的PAC-PDMDAAC()昆凝出水巾不同组分残留铝含量较低,更易降低出水中残留铝的浓度；投加量与pH值对复合混凝剂在水体中的残留铝量有一定的影响,在投加量为6-8mg／L、初始pH为7.0-8.5的条件下可有效控制净化水中残留铝含量；混凝剂混凝出水中残留铝中大部分是总溶解型铝,总溶解性铝溶解性有机铝成分最大,溶解性单体铝主要以溶解性无机单体铝为主。
5.总铝、总溶解性铝、溶解性单体铝及溶解性有机铝的浓度随混凝沉淀水力条件的变化呈现出了不同的变化规律；从残留铝含量及组分分布来看,快速搅拌强度、快搅时间、慢速搅拌强度、慢速搅拌时间和沉淀时间对水中不同组分残留铝的含量具有不同程度的影响。使用PAC和PASiC处理相应季节引黄水库水中选择快速搅拌转速为200r/min、快速搅拌时间为1min、慢速搅拌转速为40r/min、慢速搅拌时间为15min时对不同组分残留铝的控制效果最佳；使用PAC-PDMDAAC处理夏季引黄水库水巾选择快速搅拌转速为100～200r/min、快速搅拌时间为1min、慢速搅拌转速为40～50r/min、慢速搅拌时间为15～20min、时能够使PAC-PDMDAAC(?)争化后水中含有较低浓度的残留铝：相对于混凝过程,沉淀过程对残留铝组分的影响略小。综合考虑水处理工艺的实际运行情况及不同残留铝组分的浓度,在使用不同的铝盐混凝剂处理相应季节引黄水库水中应选择沉淀时间为30min较好。
6.使用同种混凝剂在不同水体pH下处理引黄水库水时存在一个最佳粒径、强度、生长速度和浊度去除率使净化后水中总铝和颗粒态铝浓度最低。复合混凝剂中MR=2：1时最佳粒径为335～347μm、最佳生长速度为35.2～35.7μm/min、最佳絮体强度为30、最适浊度去除率为75.2%-76.1%；MR=4：1时该最佳粒径为342-381μm、最佳生长速度为38.5～47.7μm/min、最佳絮体强度为26、最适浊度去除率为78.6%-80.9%；MR=8：1时该最佳粒径为278～300μm、最佳生长速度为32.1-33.7μm/min、最佳絮体强度为33、最适浊度去除率为74.6%-75.1%。在某一水体pH下采用具有不同MR值的复合混凝剂处理引黄水库水时,絮体粒径和生长速度越大、强度越低、浊度去除率越高,相应组分残留铝浓度尤其是颗粒态铝浓度越低；颗粒态铝浓度与絮体粒径或生长速度之间均呈现较明显的负线性相关性,其与絮体强度之间呈现较明显的正线性相关性；同种混凝剂下影响残留铝浓度的最主要因素是pH变化引起铝溶解度的变化；在某水体pH下采用不同MR值的混凝剂处理引黄水库水时影响铝浓度的最主要因素是混凝去除效果；溶解态有机结合部分残留铝的浓度与有机物去除率之间以及颗粒组分残留铝浓度与浊度去除率之间均呈现较弱的负线性相关性。
Based on comprehensive analysis of numerous literatures, the fractionation and measurement of residual Al speciation was determined for drinking water treatment. Effect of coagulant type, synthesis condition, coagulant dosage, initial pH and hydraulic condition on coagulation performance, residual Al concentration, residual Al speciation distribution and residual Al ratio were investigated with respect to the coagulation treatment of humic acid-kaolin simulated water and reservoir water in this research. The optimal dosage and initial pH were confirmed for coagulation of two raw waters using various Al-based coagulants from the coagulation removal performance and residual Al concentration point of view. Optimum hydraulic condition was also clarified for seasonal reservoir water treatment using Al-based coagulants. The main factors influencing residual Al content and speciation distribution were also analyzed. In addition, relationship between coagulation performance (floc operational parameters) and residual Al speciation concentration was discussed in this paper. The main conclusions were summarized as follows:
1. During humic acid-kaolin simulated water coagulation, turbidity and UV254removal efficiencies could reach about90%at the tested dosages for AICl3. Al2(SO4)3and polyaluminum chloride (PAC) coagulation. At higher dosage, PAC gave better coagulation effect. Residual total Al content and residual Al ratio of PAC (0.9mg/L and-3.0%, respectively) were greatly lower than those of AICl3and A12(SO4)3. PAC could effectively decrease the content of dissolved Al speciation (about0.6mg/L) with higher toxicity. At initial pH between6.0-7.0, turbidity removal rate of AICI3Al2(SO4)3and PAC was94%,91.5and90.5%, respectively, while UV254removal rate of AICI3, Al2(SO4)3and PAC was87%,88.5%and82%. respectively. PAC exhibited the least residual Al concentration and residual Al ratio regardless of pH variation. The optimal coagulation performance and lower residual Al content could be achieved at dosage of10～12mg/L. However, favorable pH range for efficient coagulation property and lower residual Al content was6.0-7.0and7.0～8.0. respectively. In addition, dissolved Al was the predominant content (60%-80%) in the effluent. In total dissolved Al, proportion of dissolved organic Al was markedly higher than that of other Al speciation. Dissolved nomomeric Al fraction was mainly present in dissolved inorganically bound Al.
2. With respect to the coagulation treatment of reservoir water in spring and fall, PAC had the advantages of higher coagulation removal efficiency, stronger charge neutralization ability, lower residual Al concentration, lower residual Al ratio and wider suitable pH range compared to conventional AICI3. Charge neutralization was examined to be more efficient at acid conditions for AICl3and PAC coagulation. The organic material in treated water was mostly hydrophobic, and this material was removed better with higher dosages and in neutral or weakly alkaline conditions. It was not easy for Al fraction in PAC to transfer and remain in coagulated effluent and residual Al ratio of PAC was lower than that of AICl3. However, higher dissolved organically bound Al content was achievable for PAC coagulation. Coagulation performance of PAC could be optimized at basicity (B)=2.0, dosage=12～15mg/L and pH=6.0. The majority of total Al existed most in dissolved Al form, among which, dissolved organic Al was the predominant speciation. Most dissolved monomeric Al was inorganically monomeric Al. Lower values for concentration of various residual Al species and residual Al ratio were achievable at dosage=12-15mg/L and pH=7.0～8.5. Additionally, residual Al ratio was lowest at B of2.0.
3. Adsorption bridging and sweep flocculation were main and effective mechanisms for coagulation treatment of reservoir water with low temperature and low turbidity in winter using polvaluminum silicate chloride (PASiC). With OH-/Al3-molar ratio=2.0and Si/Al molar ratio=0.05in PASiC coagulant. PASiC exhibited beneficial coagulation property and relatively lower content of residual Al. Regardless of B value and Si/Al ratio, the most efficient turbidity and organic matter removal rate were achieved at dosage of12-15mg/L and initial pH of6.0-7.0for PASiC coagulation. Yet. dosage=10～15mg/L and pH1=7.0-8.5were beneficial to the reduction of residual Al content. It was suitable for PASiC to remove macromolecular organics with hydrophobic and aromatic characteristics in reservoir water. In addition, majority of residual Al in the effluent existed in form of soluble or dissolved Al fraction. Monomeric Al was almost the major speciation in dissolved Al and dissolved inorganically-bound monomeric Al was the only component in dissolved monomeric Al. Compared to the coagulation of reservoir water in spring and fall using PAC, the optimum coagulant dosage was comparatively higher for the coagulation of reservoir water in winter using PASiC
4. With respect to the coagulation treatment of high algae-laden reservoir water in summer, coagulation characteristics of polyaluminum chloride-poly-diallyl dimethyl ammonium-chloride (PAC-PDMDAAC) were largely influenced by hydroxyl to Al molar ratio and Al to PDMDAAC mass ratio. PAC-PDMDAAC performed better coagulation performance and relatively lower residual Al speciation concentration at B=2.0and A1/PDMDAAC=4:1. The optimal coagulant dosage and initial pH for PAC-PDMDAAC coagulation were6mg/L and6.0. respectively. Concentration of various residual Al species in finished water was dramatically affected by coagulant dosage and initial pH for the composite PAC-PDMDAAC Coagulation conditions of dosage=6-8mg/L and initial pH=7.0～8.5were favorable for the control of residual Al speciation concentration. Majority of the total Al in treated water was dissolved Al. In the dissolved Al fraction, organically bound Al forms were present at a higher proportion. There existed almost no dissolved organically bound nomomeric Al fraction in treated water.
5. Concentrations of total Al, total dissolved Al, dissolved monomeric Al and dissolved organically bound Al showed different variation tendency along with the variation of hydraulic conditions during coagulation. For the coagulation treatment of reservoir water using PAC and PASiC, concentrations of various residual Al speciation could be effectively reduced at conditions of rapid mixing speed=200r/min, rapid mixing time=l min. slow mixing speed=40r/min. slow mixing time=15min and settlement time=30min. For PAC-PDMDAAC coagulation in high algae-laden reservoir water in summer, the rapid mixing speed, rapid mixing time, slow mixing speed, slow mixing time and settlement time for minimal residual Al content were 100～200r/min,1min,40～50r/min,15～20min,respectively. The effect of settlement procedure on residual Al concentration was comparatively lower compared to the coagulation process. Considering actual water treatment process and residual Al speciation concentration, settlement time should be determined at30min for seasonal reservoir water treatment using various Al-based coagulants.
6. The moderate (optimum) floc size, strength factor, growth rate and turbidity removal efficiency were favorable to the reduction of total Al and suspended Al content for one coagulant under various pH conditions. For PAC-PDMDAAC (MR=2:1) coagulation, concentration of total Al and suspended Al could be reduced effectively at floe size of335～347μm, floc growth rate of35.2～35.7μm/min,floc strength of30and turbidity removal rate of75.2%～76.1%. In case of MR=4:1,the optimum parameters for residual Al content minimization were:floc size=342～381μm, floc growth rate=8.5～47.7μm/min, floc strength=26and turbidity removal efficiency=78.6%～80.9%. In case of MR=8:1, content of of total Al and suspended Al could be minimized at floc size of278～300μm, floc growth rate of32.1～33.7μm/min, floc strength of33and turbidity removal rate of74.6%～75.1%. Under these conditions, residual Al content was mainly affected by Al solubility due to pH variation. For different coagulation system under same pH condition, comparatively lower corresponding residual Al content was achieved at larger floc size, higher floc growth rate, lower floc strength and higher turbidity removal efficiency. And residual Al concentration was primarily related to coagulation removal performance for different coagulation system under the same pH condition. Residual Al content and floc operational parameters (coagulation efficiency) exhibited a linear correlation.
1.在腐植酸-高岭土模拟地表水混凝处理中,氯化铝、硫酸铝和聚合氯化铝(PAC)在不同投加量下的浊度和UV254去除率最高可达90%左右；PAC投加量较高时混凝效果较好,其混凝出水巾残留总铝量(约为0.9mg/L)和余铝率(-3.0%)均是三种混凝剂巾最低的,且PAC能够有效降低出水巾毒性较大的溶解性铝的含量(约为0.6mg／L)；在pH为6.0-7.0之间,氯化铝、硫酸铝和PAC的浊度去除率分别可达到94%,91.5%和90.5%,UV254去除率可分别达到87%,88.5%和82%；不同pH下PAC混凝出水中残留铝含量及余铝率最低；三种混凝剂在投加量范围为10-12mg／L下处理腐植酸-高岭土模拟地表水时可以取得最佳的混凝去除效果和最低的残留铝含量；但它们取得最佳混凝效果和最低残留铝含量的pH范围分别为6.0-7.0和7.0-8.0；三种混凝剂净化后水中残留铝均大部分以溶解性总铝的形式存在(约60%-80%),溶解性有机铝在总溶解性铝巾所占比例较大,溶解性单体铝组分基本均为溶解性无机单体铝。
2.PAC更适于春秋季节引黄水库水混凝处理,不同投加量和pH下具有比传统氯化铝混凝去除率更高、电中和能力更强、残留铝含量更低、混凝剂本身余铝率更低和对水体pH改变的适应性更强的优点；氯化铝和PAC的电中和能力在酸性条件下更强,两种混凝剂混凝出水中大部分是亲水性有机物,增加投加量以及中性和偏碱性条件更利于疏水性有机物的去除；不同条件下PAC中的铝不易残留,余铝率均明显低于氯化铝的余铝率,但其混凝出水中溶解性有机结合铝含量较高；PAC在春秋季节引黄水库水处理中,取得较好混凝效果的碱化度(B)为2.0、投加量范围为12-15mg/L、初始水体pH为6.0左右；净化后水中残留铝均大部分以溶解性总铝的形式存在,且溶解性有机铝在总溶解性铝中所占比例较大,溶解性单体铝主要以溶解性无机单体铝为主；各组分残留铝浓度及混凝剂余铝率均在投加量为12～15mg/L、pH为7.0-8.5下较低,可有效控制混凝出水中的残留铝含量；此外,B值为2.0的PAC在春季水库水处理巾余铝率较低。
3.在冬季低温低浊引黄水库水处理中,聚硅氯化铝(PASiC)以吸附架桥和卷扫絮凝为主，B值为2.0、硅铝摩尔比为0.05时PASiC具有更好的混凝效果和更低的残留铝含量；不论B值和硅铝摩尔比如何变化,PASiC均在投加量范围为12-15mg/L、初始pH为6.0-7.0时对引黄水库水中的浊度和有机物具有良好的去除效果,而在投加量为10～15mg/L、初始pH为7.0-8.5下PASiC混凝后水巾含有较低浓度的残留铝；PASiC更适宜于去除水库水巾疏水性和具有芳香族特性的大分子有机物;PASiC在冬季低温低浊引黄水库水处理中,混凝出水巾残留铝中大部分是总溶解性铝,在总溶解性铝中溶解性单体铝的成分最大,溶解性单体铝主要以溶解性无机单体铝为主;同使用PAC处理春秋季引黄水库水相比,使用PASiC(?)昆凝处理冬季低温低浊引黄水库水时混凝剂的最佳投加量较高
4.在夏季高藻引黄水库水处理中,向PAC中引入聚二甲基二烯丙基氯化铵(PDMDAAC)后制备出的聚合氯化铝-聚二甲基二烯丙基氯化铵(PAC-PDMDAAC)复合混凝剂的混凝特性受无机有机组分质量比(MR值)及B值的影响,B值为2.0、MR值为4：1时复合混凝剂的混凝效果较好；PAC-PDMDAAC处理夏季高藻引黄水库水的最佳投加量为6mg/L,最佳水体pH为6.0左右；B值为2.0、MR值为4：1的PAC-PDMDAAC()昆凝出水巾不同组分残留铝含量较低,更易降低出水中残留铝的浓度；投加量与pH值对复合混凝剂在水体中的残留铝量有一定的影响,在投加量为6-8mg／L、初始pH为7.0-8.5的条件下可有效控制净化水中残留铝含量；混凝剂混凝出水中残留铝中大部分是总溶解型铝,总溶解性铝溶解性有机铝成分最大,溶解性单体铝主要以溶解性无机单体铝为主。
5.总铝、总溶解性铝、溶解性单体铝及溶解性有机铝的浓度随混凝沉淀水力条件的变化呈现出了不同的变化规律；从残留铝含量及组分分布来看,快速搅拌强度、快搅时间、慢速搅拌强度、慢速搅拌时间和沉淀时间对水中不同组分残留铝的含量具有不同程度的影响。使用PAC和PASiC处理相应季节引黄水库水中选择快速搅拌转速为200r/min、快速搅拌时间为1min、慢速搅拌转速为40r/min、慢速搅拌时间为15min时对不同组分残留铝的控制效果最佳；使用PAC-PDMDAAC处理夏季引黄水库水巾选择快速搅拌转速为100～200r/min、快速搅拌时间为1min、慢速搅拌转速为40～50r/min、慢速搅拌时间为15～20min、时能够使PAC-PDMDAAC(?)争化后水中含有较低浓度的残留铝：相对于混凝过程,沉淀过程对残留铝组分的影响略小。综合考虑水处理工艺的实际运行情况及不同残留铝组分的浓度,在使用不同的铝盐混凝剂处理相应季节引黄水库水中应选择沉淀时间为30min较好。
6.使用同种混凝剂在不同水体pH下处理引黄水库水时存在一个最佳粒径、强度、生长速度和浊度去除率使净化后水中总铝和颗粒态铝浓度最低。复合混凝剂中MR=2：1时最佳粒径为335～347μm、最佳生长速度为35.2～35.7μm/min、最佳絮体强度为30、最适浊度去除率为75.2%-76.1%；MR=4：1时该最佳粒径为342-381μm、最佳生长速度为38.5～47.7μm/min、最佳絮体强度为26、最适浊度去除率为78.6%-80.9%；MR=8：1时该最佳粒径为278～300μm、最佳生长速度为32.1-33.7μm/min、最佳絮体强度为33、最适浊度去除率为74.6%-75.1%。在某一水体pH下采用具有不同MR值的复合混凝剂处理引黄水库水时,絮体粒径和生长速度越大、强度越低、浊度去除率越高,相应组分残留铝浓度尤其是颗粒态铝浓度越低；颗粒态铝浓度与絮体粒径或生长速度之间均呈现较明显的负线性相关性,其与絮体强度之间呈现较明显的正线性相关性；同种混凝剂下影响残留铝浓度的最主要因素是pH变化引起铝溶解度的变化；在某水体pH下采用不同MR值的混凝剂处理引黄水库水时影响铝浓度的最主要因素是混凝去除效果；溶解态有机结合部分残留铝的浓度与有机物去除率之间以及颗粒组分残留铝浓度与浊度去除率之间均呈现较弱的负线性相关性。
Based on comprehensive analysis of numerous literatures, the fractionation and measurement of residual Al speciation was determined for drinking water treatment. Effect of coagulant type, synthesis condition, coagulant dosage, initial pH and hydraulic condition on coagulation performance, residual Al concentration, residual Al speciation distribution and residual Al ratio were investigated with respect to the coagulation treatment of humic acid-kaolin simulated water and reservoir water in this research. The optimal dosage and initial pH were confirmed for coagulation of two raw waters using various Al-based coagulants from the coagulation removal performance and residual Al concentration point of view. Optimum hydraulic condition was also clarified for seasonal reservoir water treatment using Al-based coagulants. The main factors influencing residual Al content and speciation distribution were also analyzed. In addition, relationship between coagulation performance (floc operational parameters) and residual Al speciation concentration was discussed in this paper. The main conclusions were summarized as follows:
1. During humic acid-kaolin simulated water coagulation, turbidity and UV254removal efficiencies could reach about90%at the tested dosages for AICl3. Al2(SO4)3and polyaluminum chloride (PAC) coagulation. At higher dosage, PAC gave better coagulation effect. Residual total Al content and residual Al ratio of PAC (0.9mg/L and-3.0%, respectively) were greatly lower than those of AICl3and A12(SO4)3. PAC could effectively decrease the content of dissolved Al speciation (about0.6mg/L) with higher toxicity. At initial pH between6.0-7.0, turbidity removal rate of AICI3Al2(SO4)3and PAC was94%,91.5and90.5%, respectively, while UV254removal rate of AICI3, Al2(SO4)3and PAC was87%,88.5%and82%. respectively. PAC exhibited the least residual Al concentration and residual Al ratio regardless of pH variation. The optimal coagulation performance and lower residual Al content could be achieved at dosage of10～12mg/L. However, favorable pH range for efficient coagulation property and lower residual Al content was6.0-7.0and7.0～8.0. respectively. In addition, dissolved Al was the predominant content (60%-80%) in the effluent. In total dissolved Al, proportion of dissolved organic Al was markedly higher than that of other Al speciation. Dissolved nomomeric Al fraction was mainly present in dissolved inorganically bound Al.
2. With respect to the coagulation treatment of reservoir water in spring and fall, PAC had the advantages of higher coagulation removal efficiency, stronger charge neutralization ability, lower residual Al concentration, lower residual Al ratio and wider suitable pH range compared to conventional AICI3. Charge neutralization was examined to be more efficient at acid conditions for AICl3and PAC coagulation. The organic material in treated water was mostly hydrophobic, and this material was removed better with higher dosages and in neutral or weakly alkaline conditions. It was not easy for Al fraction in PAC to transfer and remain in coagulated effluent and residual Al ratio of PAC was lower than that of AICl3. However, higher dissolved organically bound Al content was achievable for PAC coagulation. Coagulation performance of PAC could be optimized at basicity (B)=2.0, dosage=12～15mg/L and pH=6.0. The majority of total Al existed most in dissolved Al form, among which, dissolved organic Al was the predominant speciation. Most dissolved monomeric Al was inorganically monomeric Al. Lower values for concentration of various residual Al species and residual Al ratio were achievable at dosage=12-15mg/L and pH=7.0～8.5. Additionally, residual Al ratio was lowest at B of2.0.
3. Adsorption bridging and sweep flocculation were main and effective mechanisms for coagulation treatment of reservoir water with low temperature and low turbidity in winter using polvaluminum silicate chloride (PASiC). With OH-/Al3-molar ratio=2.0and Si/Al molar ratio=0.05in PASiC coagulant. PASiC exhibited beneficial coagulation property and relatively lower content of residual Al. Regardless of B value and Si/Al ratio, the most efficient turbidity and organic matter removal rate were achieved at dosage of12-15mg/L and initial pH of6.0-7.0for PASiC coagulation. Yet. dosage=10～15mg/L and pH1=7.0-8.5were beneficial to the reduction of residual Al content. It was suitable for PASiC to remove macromolecular organics with hydrophobic and aromatic characteristics in reservoir water. In addition, majority of residual Al in the effluent existed in form of soluble or dissolved Al fraction. Monomeric Al was almost the major speciation in dissolved Al and dissolved inorganically-bound monomeric Al was the only component in dissolved monomeric Al. Compared to the coagulation of reservoir water in spring and fall using PAC, the optimum coagulant dosage was comparatively higher for the coagulation of reservoir water in winter using PASiC
4. With respect to the coagulation treatment of high algae-laden reservoir water in summer, coagulation characteristics of polyaluminum chloride-poly-diallyl dimethyl ammonium-chloride (PAC-PDMDAAC) were largely influenced by hydroxyl to Al molar ratio and Al to PDMDAAC mass ratio. PAC-PDMDAAC performed better coagulation performance and relatively lower residual Al speciation concentration at B=2.0and A1/PDMDAAC=4:1. The optimal coagulant dosage and initial pH for PAC-PDMDAAC coagulation were6mg/L and6.0. respectively. Concentration of various residual Al species in finished water was dramatically affected by coagulant dosage and initial pH for the composite PAC-PDMDAAC Coagulation conditions of dosage=6-8mg/L and initial pH=7.0～8.5were favorable for the control of residual Al speciation concentration. Majority of the total Al in treated water was dissolved Al. In the dissolved Al fraction, organically bound Al forms were present at a higher proportion. There existed almost no dissolved organically bound nomomeric Al fraction in treated water.
5. Concentrations of total Al, total dissolved Al, dissolved monomeric Al and dissolved organically bound Al showed different variation tendency along with the variation of hydraulic conditions during coagulation. For the coagulation treatment of reservoir water using PAC and PASiC, concentrations of various residual Al speciation could be effectively reduced at conditions of rapid mixing speed=200r/min, rapid mixing time=l min. slow mixing speed=40r/min. slow mixing time=15min and settlement time=30min. For PAC-PDMDAAC coagulation in high algae-laden reservoir water in summer, the rapid mixing speed, rapid mixing time, slow mixing speed, slow mixing time and settlement time for minimal residual Al content were 100～200r/min,1min,40～50r/min,15～20min,respectively. The effect of settlement procedure on residual Al concentration was comparatively lower compared to the coagulation process. Considering actual water treatment process and residual Al speciation concentration, settlement time should be determined at30min for seasonal reservoir water treatment using various Al-based coagulants.
6. The moderate (optimum) floc size, strength factor, growth rate and turbidity removal efficiency were favorable to the reduction of total Al and suspended Al content for one coagulant under various pH conditions. For PAC-PDMDAAC (MR=2:1) coagulation, concentration of total Al and suspended Al could be reduced effectively at floe size of335～347μm, floc growth rate of35.2～35.7μm/min,floc strength of30and turbidity removal rate of75.2%～76.1%. In case of MR=4:1,the optimum parameters for residual Al content minimization were:floc size=342～381μm, floc growth rate=8.5～47.7μm/min, floc strength=26and turbidity removal efficiency=78.6%～80.9%. In case of MR=8:1, content of of total Al and suspended Al could be minimized at floc size of278～300μm, floc growth rate of32.1～33.7μm/min, floc strength of33and turbidity removal rate of74.6%～75.1%. Under these conditions, residual Al content was mainly affected by Al solubility due to pH variation. For different coagulation system under same pH condition, comparatively lower corresponding residual Al content was achieved at larger floc size, higher floc growth rate, lower floc strength and higher turbidity removal efficiency. And residual Al concentration was primarily related to coagulation removal performance for different coagulation system under the same pH condition. Residual Al content and floc operational parameters (coagulation efficiency) exhibited a linear correlation.
引文
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