形态特征及藻源有机质对改性粘土絮凝有害藻华生物效率的影响
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摘要
改性粘土技术是当前国内外最受关注的有害藻华应急治理方法，多次的现场成功应用证明了该技术和方法的有效性和可行性。如何进一步提高改性粘土消除藻华生物的效率仍是当前改性粘土研究的重点，而开展粘土与藻华生物的分形絮凝机制研究将为提高粘土/改性粘土对有害藻华生物絮凝效率提供理论指导。现阶段研究粘土絮凝去除藻华的传统理论，一方面将颗粒简化为规则的几何图形，忽略了颗粒形态特征的影响；另一方面也没有考虑藻华水体内大量微藻产生的藻源有机质对絮凝过程的影响。而大量研究已证明，水体中的颗粒形态及有机大分子对于颗粒的絮凝过程有重要影响。
本文基于分形和吸附的相关理论，研究了改性粘土絮凝有害藻华生物过程中各种颗粒物的形态学特征，考察了藻源有机质在改性粘土上的吸附特性及藻源有机质对微藻细胞、改性粘土颗粒、微藻-粘土絮体形态特征的影响；利用图像分析法，测定了絮凝体的分形维数，并借助分形维数半定量化分析了絮凝体的形态学特征；进而分析了粘土-微藻絮凝体的分形变化特征及其影响因素；获得了粘土颗粒絮凝有害藻华生物的关键影响因子，为进一步提高改性粘土治理有害藻华的絮凝效率提供理论依据。本研究的主要结果如下：
改性粘土及藻华生物形态学特征研究。PAC改性剂浓度、pH和离子强度对粘土絮凝体的形态特征具有重要影响。PAC改性剂能有效提高粘土絮凝体的分形维数，最佳改性比例是粘土/改性剂为10:1；最佳絮凝pH范围为6-7；离子强度可以提高絮凝体的分形维数和致密性。絮凝体分形维数能够较为准确得到絮凝体形态的即时变化特征，是深入了解絮凝体的生长机制的较为理想的形态学指标。不同藻华生物在不同生长期有不同的形态特征和分形维数；指数期的东海原甲藻、中肋骨条藻和稳定期的赤潮异弯藻细胞的分形维数较大，分别为1.6785,1.7766和1.6757。
藻源有机质对改性粘土絮凝效率的影响。分别以海藻酸钠、氨基酸为藻源有机质不同组分的模式化合物，考察了藻源有机质与改性粘土的相互作用机制及其影响因素。结果表明：藻源有机质在改性粘土上的吸附是一个自发的、复杂的、同时受膜扩散吸附和粒子内部扩散吸附控制的过程，其受到改性剂浓度、pH和离子强度的重要影响；其中，改性剂最佳改性比例为5%。藻源有机质在改性粘土上的吸附动力学符合伪二阶动力学模型(pseudo-second order model)，而热力学研究表明海藻酸钠在改性粘土上的吸附符合Freundlich和Langmuir吸附等温线，氨基酸在改性粘土的吸附等温线属于C型等温线。藻源有机质对改性粘土絮凝速率及絮凝体特征具有显著的影响，当海藻酸钠浓度在10-100mg/L范围内时,可以提高改性黏土絮凝的速率，絮凝体的分形维数、絮凝体强度呈现出先增大后减小的规律;其中,最佳浓度为50mg/L,其最大絮凝速率达到44.13%、分形维数为1.6823。低浓度（<10mg/L）组海藻酸钠不利于改性粘土颗粒间的絮凝，高浓度的（>100mg/L）海藻酸钠能促进改性粘土的絮凝效率，但促进作用呈现减小的趋势。对于氨基酸化合物，改性粘土颗粒絮凝体分形维数均大于未改性粘土组；在一定浓度范围内，氨基酸化合物促粘土颗粒形成较为致密、空隙率较低的絮凝体；表现为分形维数增大。
粘土-微藻絮凝特征及其影响因素研究。粘土-微藻絮凝体分形维数、粘土絮凝去除藻华生物的能力均随着改性剂比例的增大呈现出逐渐增大的趋势；絮体分形维数与去除率RE相关性分析表明，粘土-微藻絮凝体分形维数的变化对絮凝效率的变化具有较好的指示作用。不同生物学特征的3种微藻的藻细胞形态特征、藻液内不同大小有机颗粒物对改性粘土絮凝速率有不同的影响。改性粘土对不同生长期的塔玛亚历山大藻液、藻细胞再悬浮液表现出不同的去除能力：对于藻液的去除率为迟滞期>衰亡期>稳定期>指数期；对于藻细胞再悬浮液，指数期的去除率最小，但各个时期的差异性没有藻液显著。藻液中的有机质TON/TOP/TOC随着塔玛亚历山大藻的生长呈现出不同的变化趋势。有机质浓度与藻细胞再悬浮液和藻液二者之间的去除率差值dRE的相关性分析表明，TON与dRE之间没有明显的相关关系；低浓度的TOC(≤1.0mmolC/L)与dRE呈现出较好的正相关性，表明较低浓度的TOC可以降低改性粘土对有害藻华生物的絮凝去除效率。
Modified clay was a promising method for mitigation of harmful algalblooms.The morphology of flocs and algal orianic materials (AOMs) were key factorsaffecting the removal efficiency (RE) of modified clays for HAB organisms. Thisstudy was conducted to investigate the effects of morphology of aggregates andAOMs on HAB cells removal using modified clays. Kaolinite modified withpolyaluminium chloride (PAC) was used as modified clay model substances. REs ofdifferent HAB species were determined and the fractal dimensions of HAB cell,clay-clay and algae-clay units, were assessed by non-intrusive optical sampling anddigital image analysis techniques, in different experiments, respectively. Experimentswere also carried out to study the mutual effect between AOMs and modified calys,for better understanding of the mechanisms and factors affecting the adsorption ofAOMs onto modified clays and the effect of AOMs on the coagulation rate and flocsformation of modified clays. Furthermore, the relation between the fractal dimensionsand REs, AOMs and REs, were analyzed, respectively. The main results were asfollows:
The morphological characteristics of clay and algal cell were studied in this test.The results showed that the fractal dimensions of clay-clay flocs were affectedmarkedly by modifier dosage, pH and ionic strength. Compared with original clay, theflocs of modified clay was with a higher fractal dimension, which reflected the morecompact flocs. The optimum mass ratio between clay and modifier was10:1. Theflocs fractal dimension increased with increasing ionic strength, where the similartrend was found at pH<7, but the opposite was true above pH7. Thus, the optimumpH range for clay-clay aggregation was6-7. Furthermore, the fractal dimension was abetter indicater of the instant variation of flocs morphology. The fractal dimension ofalgal cell was determined by the algal species and its growth phase, e.g. the cells of P.donghaiense and S.costatum with a higher fractal dimension were in theirexponential phase, while H.akshiwo was in its stable phase, and the values were1.6785,1.7766and1.6757, respectively.
In order to investigate the mutual effect between AOMs and modified calys, weused sodium alginate and amino acid as AOMs different component model substances.The adsorption of AOMs on modified clays was studied as a function of modifierdosage, contact time, solution pH and ionic strength through batch adsorptionexperiments. Kinetics revealed that the AOMs adsorption rate was described well by apseudo-second order model. Modifier effectively enhanced the adsorption capacity ofkaolinite and increased the adsorption rate, and the optimum additive amount ofmodifier was5%. The adsorption thermodynamics for AOMs onto modified clayssuggests that AOMs adsorption is a spontaneous process. The experimental data fittedboth the Freundlich and Langmuir adsorption equations well for alginate and was welldescribed by C isotherm curve for amino acid. The adsorption of AOMs ontomodified clays was highly dependent on pH and ionic strength. The effect of AOMson the coagulation rate and flocs formation of modified clay was also investigated.The flocculation kinetics of modified clay particles at various concentrations ofsodium alginate solutions were studied. And the flocs fractal dimension wascalculated by image analysis software. Our results indicate that the coagulation rate ofmodified clay and the fractal dimension of flocs were lower than that of control whenthe concentration of sodium alginate is below10mg/L. In the range of10-100mg/L,sodium alginate can improve the coagulation rate of modified clay; the flocs fractaldimension and flocs strength increased steadily to a peak and then decreased. Theoptimum concentration of sodium alginate was50mg/L, along with the maximumcoagulation rate of44.13%and the flocs dimension of1.6823respectively. However,the flocs fractal dimension and coagulation rate decreased when the concentration ofsodium alginate was higher than100mg/L, resulting in subsequent increase of theflocs voidage. For amino acid, in a certain concentration rang, the fractal dimensionsof flocs increased with the concentration of amino acid increasing, which reflectedmore compact and lower voidage flocs. In addition, the fractal dimension of modifiedclay was higer than original clay’s.
Finally, the morphology of algae-clay and its effect on the RE of HAB organisms,the variation characteristics of AOMs in algal growth phase and its effect on REs,were studied. The fractal dimensions of algae-clay and REs were both increase with the increase of modifier dosage. The relation between the fractal dimensions and REssuggested that the fractal dimension can effectively indicate the variation of REs. Theimpacts of different component of algal suspensions were different. The REs ofA.tamarense cell in suspensions by modified clays in different growth pahse were: lagphase> decline phase>stable phase>exponential phase. For cell resuspensions, thelowest RE was in exponential phase, however, there was no significant differencebetween the phases. The different component of AOMs, such as TON, TOP, TOC,showed different trend with A.tamarense growth. The relation between AOMs and dRE,which was the difference between REs of algal cell resuspension and algal suspension,was analysed and the result showed that there was no significant relation betweenTON and dRE, but a stronger positive correlation between the lower concertration ofTOC (≤1.0mmolC/L) and dRE. It indicated that a lower concertration of TOC wouldreduce the flocculation effect of modified clay on HAB organisms.
本文基于分形和吸附的相关理论，研究了改性粘土絮凝有害藻华生物过程中各种颗粒物的形态学特征，考察了藻源有机质在改性粘土上的吸附特性及藻源有机质对微藻细胞、改性粘土颗粒、微藻-粘土絮体形态特征的影响；利用图像分析法，测定了絮凝体的分形维数，并借助分形维数半定量化分析了絮凝体的形态学特征；进而分析了粘土-微藻絮凝体的分形变化特征及其影响因素；获得了粘土颗粒絮凝有害藻华生物的关键影响因子，为进一步提高改性粘土治理有害藻华的絮凝效率提供理论依据。本研究的主要结果如下：
改性粘土及藻华生物形态学特征研究。PAC改性剂浓度、pH和离子强度对粘土絮凝体的形态特征具有重要影响。PAC改性剂能有效提高粘土絮凝体的分形维数，最佳改性比例是粘土/改性剂为10:1；最佳絮凝pH范围为6-7；离子强度可以提高絮凝体的分形维数和致密性。絮凝体分形维数能够较为准确得到絮凝体形态的即时变化特征，是深入了解絮凝体的生长机制的较为理想的形态学指标。不同藻华生物在不同生长期有不同的形态特征和分形维数；指数期的东海原甲藻、中肋骨条藻和稳定期的赤潮异弯藻细胞的分形维数较大，分别为1.6785,1.7766和1.6757。
藻源有机质对改性粘土絮凝效率的影响。分别以海藻酸钠、氨基酸为藻源有机质不同组分的模式化合物，考察了藻源有机质与改性粘土的相互作用机制及其影响因素。结果表明：藻源有机质在改性粘土上的吸附是一个自发的、复杂的、同时受膜扩散吸附和粒子内部扩散吸附控制的过程，其受到改性剂浓度、pH和离子强度的重要影响；其中，改性剂最佳改性比例为5%。藻源有机质在改性粘土上的吸附动力学符合伪二阶动力学模型(pseudo-second order model)，而热力学研究表明海藻酸钠在改性粘土上的吸附符合Freundlich和Langmuir吸附等温线，氨基酸在改性粘土的吸附等温线属于C型等温线。藻源有机质对改性粘土絮凝速率及絮凝体特征具有显著的影响，当海藻酸钠浓度在10-100mg/L范围内时,可以提高改性黏土絮凝的速率，絮凝体的分形维数、絮凝体强度呈现出先增大后减小的规律;其中,最佳浓度为50mg/L,其最大絮凝速率达到44.13%、分形维数为1.6823。低浓度（<10mg/L）组海藻酸钠不利于改性粘土颗粒间的絮凝，高浓度的（>100mg/L）海藻酸钠能促进改性粘土的絮凝效率，但促进作用呈现减小的趋势。对于氨基酸化合物，改性粘土颗粒絮凝体分形维数均大于未改性粘土组；在一定浓度范围内，氨基酸化合物促粘土颗粒形成较为致密、空隙率较低的絮凝体；表现为分形维数增大。
粘土-微藻絮凝特征及其影响因素研究。粘土-微藻絮凝体分形维数、粘土絮凝去除藻华生物的能力均随着改性剂比例的增大呈现出逐渐增大的趋势；絮体分形维数与去除率RE相关性分析表明，粘土-微藻絮凝体分形维数的变化对絮凝效率的变化具有较好的指示作用。不同生物学特征的3种微藻的藻细胞形态特征、藻液内不同大小有机颗粒物对改性粘土絮凝速率有不同的影响。改性粘土对不同生长期的塔玛亚历山大藻液、藻细胞再悬浮液表现出不同的去除能力：对于藻液的去除率为迟滞期>衰亡期>稳定期>指数期；对于藻细胞再悬浮液，指数期的去除率最小，但各个时期的差异性没有藻液显著。藻液中的有机质TON/TOP/TOC随着塔玛亚历山大藻的生长呈现出不同的变化趋势。有机质浓度与藻细胞再悬浮液和藻液二者之间的去除率差值dRE的相关性分析表明，TON与dRE之间没有明显的相关关系；低浓度的TOC(≤1.0mmolC/L)与dRE呈现出较好的正相关性，表明较低浓度的TOC可以降低改性粘土对有害藻华生物的絮凝去除效率。
Modified clay was a promising method for mitigation of harmful algalblooms.The morphology of flocs and algal orianic materials (AOMs) were key factorsaffecting the removal efficiency (RE) of modified clays for HAB organisms. Thisstudy was conducted to investigate the effects of morphology of aggregates andAOMs on HAB cells removal using modified clays. Kaolinite modified withpolyaluminium chloride (PAC) was used as modified clay model substances. REs ofdifferent HAB species were determined and the fractal dimensions of HAB cell,clay-clay and algae-clay units, were assessed by non-intrusive optical sampling anddigital image analysis techniques, in different experiments, respectively. Experimentswere also carried out to study the mutual effect between AOMs and modified calys,for better understanding of the mechanisms and factors affecting the adsorption ofAOMs onto modified clays and the effect of AOMs on the coagulation rate and flocsformation of modified clays. Furthermore, the relation between the fractal dimensionsand REs, AOMs and REs, were analyzed, respectively. The main results were asfollows:
The morphological characteristics of clay and algal cell were studied in this test.The results showed that the fractal dimensions of clay-clay flocs were affectedmarkedly by modifier dosage, pH and ionic strength. Compared with original clay, theflocs of modified clay was with a higher fractal dimension, which reflected the morecompact flocs. The optimum mass ratio between clay and modifier was10:1. Theflocs fractal dimension increased with increasing ionic strength, where the similartrend was found at pH<7, but the opposite was true above pH7. Thus, the optimumpH range for clay-clay aggregation was6-7. Furthermore, the fractal dimension was abetter indicater of the instant variation of flocs morphology. The fractal dimension ofalgal cell was determined by the algal species and its growth phase, e.g. the cells of P.donghaiense and S.costatum with a higher fractal dimension were in theirexponential phase, while H.akshiwo was in its stable phase, and the values were1.6785,1.7766and1.6757, respectively.
In order to investigate the mutual effect between AOMs and modified calys, weused sodium alginate and amino acid as AOMs different component model substances.The adsorption of AOMs on modified clays was studied as a function of modifierdosage, contact time, solution pH and ionic strength through batch adsorptionexperiments. Kinetics revealed that the AOMs adsorption rate was described well by apseudo-second order model. Modifier effectively enhanced the adsorption capacity ofkaolinite and increased the adsorption rate, and the optimum additive amount ofmodifier was5%. The adsorption thermodynamics for AOMs onto modified clayssuggests that AOMs adsorption is a spontaneous process. The experimental data fittedboth the Freundlich and Langmuir adsorption equations well for alginate and was welldescribed by C isotherm curve for amino acid. The adsorption of AOMs ontomodified clays was highly dependent on pH and ionic strength. The effect of AOMson the coagulation rate and flocs formation of modified clay was also investigated.The flocculation kinetics of modified clay particles at various concentrations ofsodium alginate solutions were studied. And the flocs fractal dimension wascalculated by image analysis software. Our results indicate that the coagulation rate ofmodified clay and the fractal dimension of flocs were lower than that of control whenthe concentration of sodium alginate is below10mg/L. In the range of10-100mg/L,sodium alginate can improve the coagulation rate of modified clay; the flocs fractaldimension and flocs strength increased steadily to a peak and then decreased. Theoptimum concentration of sodium alginate was50mg/L, along with the maximumcoagulation rate of44.13%and the flocs dimension of1.6823respectively. However,the flocs fractal dimension and coagulation rate decreased when the concentration ofsodium alginate was higher than100mg/L, resulting in subsequent increase of theflocs voidage. For amino acid, in a certain concentration rang, the fractal dimensionsof flocs increased with the concentration of amino acid increasing, which reflectedmore compact and lower voidage flocs. In addition, the fractal dimension of modifiedclay was higer than original clay’s.
Finally, the morphology of algae-clay and its effect on the RE of HAB organisms,the variation characteristics of AOMs in algal growth phase and its effect on REs,were studied. The fractal dimensions of algae-clay and REs were both increase with the increase of modifier dosage. The relation between the fractal dimensions and REssuggested that the fractal dimension can effectively indicate the variation of REs. Theimpacts of different component of algal suspensions were different. The REs ofA.tamarense cell in suspensions by modified clays in different growth pahse were: lagphase> decline phase>stable phase>exponential phase. For cell resuspensions, thelowest RE was in exponential phase, however, there was no significant differencebetween the phases. The different component of AOMs, such as TON, TOP, TOC,showed different trend with A.tamarense growth. The relation between AOMs and dRE,which was the difference between REs of algal cell resuspension and algal suspension,was analysed and the result showed that there was no significant relation betweenTON and dRE, but a stronger positive correlation between the lower concertration ofTOC (≤1.0mmolC/L) and dRE. It indicated that a lower concertration of TOC wouldreduce the flocculation effect of modified clay on HAB organisms.
引文
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