壳聚糖复合剂在水处理中的净化效能研究
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摘要
在当前的环境治理尤其在废水处理中,天然无毒的高分子有机化合物壳聚糖的使用成为人们研究的热点。本论文制备了几种壳聚糖复合剂,研究其吸附性能和机理,并利用壳聚糖优良的吸附和絮凝的特性,与无机混凝剂复配,考察它在给水处理及污泥脱水上的应用。
壳聚糖(CTS)是甲壳素脱乙酰基后的产物,制备原料丰富、无毒、易于生物降解。壳聚糖分子中丰富的氨基和羟基,具有较强的吸附、配位作用,壳聚糖复合吸附剂具有吸附染料分子、金属离子和蛋白质分子的能力。壳聚糖分子中存在游离氨基,在稀溶液中被质子化,使分子链上带大量正电荷,成为一种典型的阳离子絮凝剂,它兼有电中和和吸附絮凝的双重作用,即高分子链上的阳离子活性基团与带负电荷的胶体微粒相互吸引,降低中和胶体微粒的表面电荷,同时压缩了扩散层而使胶体微粒脱稳,并借助高分子链的吸附粘结和架桥作用而产生絮凝沉降。
水溶性染料一般都是极难降解的小分子有机物,常用的生物法处理、氧化处理效果不好,或不易操作。分别以膨润土和珍珠岩粉为载体,负载1%质量分数的壳聚糖或羧甲基壳聚糖,制得的复合吸附剂均对活性染料具有一定的脱色效果,其中膨润土负载壳聚糖吸附剂对活性大红B-3G、活性深兰B-2GLN、活性黑B-GRFN、活性墨绿B-4BLN四种染料饱和吸附量分别为:11.850mg·g~(-1)、7.760mg·g~(-1)、7.276mg·g~(-1)、8.362mg·g~(-1),高于珍珠岩粉吸附剂,并且其等温吸附曲线更符合Langmuir模型,为利用天然硅铝矿原位修复染料污染土壤提供了理论依据。负载羧甲基壳聚糖对染料的吸附容量最大,但价格较高。另外,实验表明纤维素复合壳聚糖吸附剂对酸性大红具有很好的吸附性能,吸附速度比较快,对该吸附动力学曲线利用一级吸附动力学Lagergren方程进行拟合,求得一级速率常数为0.884 h~(-1)。
通过用自制的珠状凝胶壳聚糖树脂对牛血清白蛋白的吸附实验可知,pH值、反应时间、投加量及离子强度对蛋白吸附量有影响。对水中Cd~(2+)、Al~(3+)的吸附试验表明,对水中Cd~(2+)、Al~(3+)的吸附容量分别是254.5mg·g~(-1)、49.0mg·g~(-1)。吸附的本质是配位反应,通过红外光谱、光电子光谱法表征,CTS-Cd(Ⅱ)配合物的结构是1个Cd~(2+)与壳聚糖分子中的两个氨基上的N原子、两个羟基上的O原子形成4个配位键结构的配合物,对Al~(3+)的吸附是壳聚糖通过氨基上的N原子和Al~(3+)配位。
分别以高岭土模拟水样和黄河预沉后的原水为目标水样,考察壳聚糖助凝效果。通过对模拟水样的正交实验,确定影响混凝效果的主次因素顺序和水力条件;通过对黄河预沉后的原水的絮凝实验,分析了PAC投加量、CTS投加量、pH值、CTS分子量等因素对水中浊度、COD_(Mn)去除率的影响,并与活性硅酸的助凝作用进行了对比,结果表明聚合铝PAC和壳聚糖CTS具有协同作用,PAC投加量35mg·L~(-1),CTS投加量0.15mg·L~(-1),壳聚糖助凝效果显著,浊度和有机物的去除均明显提高。通过测定絮凝过程中的Zeta电位变化曲线,说明壳聚糖溶液在pH=3-8的范围内均能保持正电性,在一定浓度的范围里,Zeta电位几乎不变,表明壳聚糖的絮凝以吸附架桥为主,电性中和为次。利用扫描电镜观察了絮体的结构形貌,通过显微摄像系统及图像分析系统观察了CTS助凝前后絮体的形态,通过双对数法计算了单加PAC、PAC/CTS复合絮凝处理水样后絮体的分形维数分别为1.294和1.385。
试验过程中设计一套测定污泥比阻的装置,通过试验发现,聚合铝PAC、壳聚糖CTS对活性污泥都有调理作用,均能改善污泥的脱水性能。考虑到壳聚糖的价格较高,将二者复合使用,能够更好的发挥无机和有机絮凝剂的优点又避免了两者的不足,污泥比阻最先达到低点,滤速较快而且有助于减少金属污泥的生成。对水厂排泥水污泥进行脱水干化处理时,选择粉煤灰作调理剂为好。
Nowadays, Chitosan as a non-toxic natural amino polymer functional material, have been applied gradually gained popularity in waste water treatment. This paper has researched the remove efficiency of pollutant using some new composite chitosan adsorbents and introduces the research and application of Chitosan on environmental pollution regulation in drinking water treatment and sludge dewatering.
Chitosan(CTS) is obtained by deacetylation of Chitin which is extracted from crustacean or from fungal biomass. Chitosan is a biodegradable, non-toxic, linear cationic polymer of high molecular weight and is a potent coagulant .Because a amount of dissociate amino groups exist chitosan macromolecule chain and it can be proton change in acidic solution. The high proportion of amine functions in this natural polymer results in novel binding properties for some kinds of dyestuffs, metal ions and protein. Chitosan was regarded as an amino polysaccharide and a soluble cationic coagulant. These cationic groups and negative ion colloid particulate attract each other and neutralize colloid surface charge. Because of the more coiled structure, chitosan polymer is able to compress pervation layer to take steady.In virtue of charge neutralization and adsorption and bridge connection effect so as to produce larger and denser flocs and affluent–NH_2 and–OH was used as absorbent for heavy metals.
Technologies for dye removal have been investigated, such as the electrolysis coagulation, chemical oxygenation, those processed condition is strict, the stability is bad. The article intends to introduce the authors’experimental study on four kinds of adsorbents which are made by chitosan-coated bentonite , chitosan-coated pearl, carboxymethyl chitosan-coated bentonite and carboxymethyl chitosan-coated pearl .The ability of chitosan-coated bentonite for the removal of reactive dye ,namely reactive red B-3G, blue B-2GLN, black B-GRFN, green B-4BLN,from aqueous solution has been studied. The experimental equilibrium data have been analyzed using the linearized forms of Langmuir, Freundlich isotherms .The Langmuir isotherm was found to provide the best theoretical correlation of the experimental data for the adsorption of all four reactive dyes. The monolayer adsorption capacities were determined to be11.850、7.760、7.276、8.362mg of dye per gram of chitosan-coated bentoniteadsorbent,respectively to four dyes. The results would provide a theoretical basisfor utilizing natural material to extract heavy metals from the contaminated soils.The adsorption of dyes onto Carboxymethyl chitosan adsorbent was expensiveprocess with high capacities. The paper also studied the application of adsorptionof Acid Brilliant Scarlet GR onto Chitosan-coated cellulose adsorbent has beenstudied. It was a fast process and K_1=0.884 h~(-1). in Lagergren equation.
The adsorption of BSA onto sphere Chitosan polymer has been experimented.Effect of amount of agents, pH value, adsorption time and ionic strength werestudied. The research results for coagulation of dairy producted wastewatersshow that the recovery efficiency of protein by chitosan was efficient. Theexperience of adsorption of Cd~(2+) and Al(Ⅲ)showed that the adsorption was a fastprocess with 254.5mg·g~(-1),49.0mg·g~(-1).capacity. Chitosan-Cd(Ⅱ), Chitosan- Al(Ⅲ)PPwas synthesized and FTIR, XPS analysis indicates that the adsorption was thecoordination of -NHB2 Band -OH groups of Chitosan to Cd~(2+).
The study assessed the feasibility of the application of chitosan for thecoagulation of kaolinite colloidal particles. The pH effect on the coagulationefficiency of chitosan is insignificant. The evidence infers that chargeneutralization is not a major mechanism controlling the formtion of floc forchitosan coagulation and the water conservancy condition is the key factorcongealed. Chitosan was used to enhance the flocculation treatment of thesurface water，which is the raw water of Yellow River in Zheng Zhou bypolymeric aluminum chloride (PAC).The improvement of removal efficiency ofturbidity and COD indicated that chitosan could enhance the flocculationtreatmen by PAC significantly. When PAC dosage is 35 mg·l~(-1), CTS dosage is0.15 mg·l~(-1), the effect of flocculation is better. Zeta potential instrument andScanning electron microscope were used to test Zeta potential and observe thestructure of flocs and infer flocculation mechanism was interpartical bridgingrather than the electrical neutralization by prositive charge. The floc wasobserved with microscope and image analysis system and the result show thatvariation in fractal dimension can make good response to flocculation level andPAC,PAC/CTS was 1.294,1.385 respectively.
The effect of the dosage of flocculants on activated sludge dewatering is analyzed through the determination of sludge specific resistance to filtration . Sludge dewatering behaviors conditioned on PAC, CTS and composite flocculants have been compared. The results show all the conditioning agent have help to sludge dewatering .Compared with Polymeric aluminum , Chitosan and PAC/CTS composite coagulant, the optimum coagulant with its optimum dosage is obtained . PAC/CTS can greatly reduce the sludge specific resistance and improves the sludge dewatering performance largely while the clarity of the filtrate was high. While designing the dewatering and drying process of sludge water from water works, we can ignore the coagulation process, and utilize fly ash of power plant as the conditioner of sludge from water works directly.
壳聚糖(CTS)是甲壳素脱乙酰基后的产物,制备原料丰富、无毒、易于生物降解。壳聚糖分子中丰富的氨基和羟基,具有较强的吸附、配位作用,壳聚糖复合吸附剂具有吸附染料分子、金属离子和蛋白质分子的能力。壳聚糖分子中存在游离氨基,在稀溶液中被质子化,使分子链上带大量正电荷,成为一种典型的阳离子絮凝剂,它兼有电中和和吸附絮凝的双重作用,即高分子链上的阳离子活性基团与带负电荷的胶体微粒相互吸引,降低中和胶体微粒的表面电荷,同时压缩了扩散层而使胶体微粒脱稳,并借助高分子链的吸附粘结和架桥作用而产生絮凝沉降。
水溶性染料一般都是极难降解的小分子有机物,常用的生物法处理、氧化处理效果不好,或不易操作。分别以膨润土和珍珠岩粉为载体,负载1%质量分数的壳聚糖或羧甲基壳聚糖,制得的复合吸附剂均对活性染料具有一定的脱色效果,其中膨润土负载壳聚糖吸附剂对活性大红B-3G、活性深兰B-2GLN、活性黑B-GRFN、活性墨绿B-4BLN四种染料饱和吸附量分别为:11.850mg·g~(-1)、7.760mg·g~(-1)、7.276mg·g~(-1)、8.362mg·g~(-1),高于珍珠岩粉吸附剂,并且其等温吸附曲线更符合Langmuir模型,为利用天然硅铝矿原位修复染料污染土壤提供了理论依据。负载羧甲基壳聚糖对染料的吸附容量最大,但价格较高。另外,实验表明纤维素复合壳聚糖吸附剂对酸性大红具有很好的吸附性能,吸附速度比较快,对该吸附动力学曲线利用一级吸附动力学Lagergren方程进行拟合,求得一级速率常数为0.884 h~(-1)。
通过用自制的珠状凝胶壳聚糖树脂对牛血清白蛋白的吸附实验可知,pH值、反应时间、投加量及离子强度对蛋白吸附量有影响。对水中Cd~(2+)、Al~(3+)的吸附试验表明,对水中Cd~(2+)、Al~(3+)的吸附容量分别是254.5mg·g~(-1)、49.0mg·g~(-1)。吸附的本质是配位反应,通过红外光谱、光电子光谱法表征,CTS-Cd(Ⅱ)配合物的结构是1个Cd~(2+)与壳聚糖分子中的两个氨基上的N原子、两个羟基上的O原子形成4个配位键结构的配合物,对Al~(3+)的吸附是壳聚糖通过氨基上的N原子和Al~(3+)配位。
分别以高岭土模拟水样和黄河预沉后的原水为目标水样,考察壳聚糖助凝效果。通过对模拟水样的正交实验,确定影响混凝效果的主次因素顺序和水力条件;通过对黄河预沉后的原水的絮凝实验,分析了PAC投加量、CTS投加量、pH值、CTS分子量等因素对水中浊度、COD_(Mn)去除率的影响,并与活性硅酸的助凝作用进行了对比,结果表明聚合铝PAC和壳聚糖CTS具有协同作用,PAC投加量35mg·L~(-1),CTS投加量0.15mg·L~(-1),壳聚糖助凝效果显著,浊度和有机物的去除均明显提高。通过测定絮凝过程中的Zeta电位变化曲线,说明壳聚糖溶液在pH=3-8的范围内均能保持正电性,在一定浓度的范围里,Zeta电位几乎不变,表明壳聚糖的絮凝以吸附架桥为主,电性中和为次。利用扫描电镜观察了絮体的结构形貌,通过显微摄像系统及图像分析系统观察了CTS助凝前后絮体的形态,通过双对数法计算了单加PAC、PAC/CTS复合絮凝处理水样后絮体的分形维数分别为1.294和1.385。
试验过程中设计一套测定污泥比阻的装置,通过试验发现,聚合铝PAC、壳聚糖CTS对活性污泥都有调理作用,均能改善污泥的脱水性能。考虑到壳聚糖的价格较高,将二者复合使用,能够更好的发挥无机和有机絮凝剂的优点又避免了两者的不足,污泥比阻最先达到低点,滤速较快而且有助于减少金属污泥的生成。对水厂排泥水污泥进行脱水干化处理时,选择粉煤灰作调理剂为好。
Nowadays, Chitosan as a non-toxic natural amino polymer functional material, have been applied gradually gained popularity in waste water treatment. This paper has researched the remove efficiency of pollutant using some new composite chitosan adsorbents and introduces the research and application of Chitosan on environmental pollution regulation in drinking water treatment and sludge dewatering.
Chitosan(CTS) is obtained by deacetylation of Chitin which is extracted from crustacean or from fungal biomass. Chitosan is a biodegradable, non-toxic, linear cationic polymer of high molecular weight and is a potent coagulant .Because a amount of dissociate amino groups exist chitosan macromolecule chain and it can be proton change in acidic solution. The high proportion of amine functions in this natural polymer results in novel binding properties for some kinds of dyestuffs, metal ions and protein. Chitosan was regarded as an amino polysaccharide and a soluble cationic coagulant. These cationic groups and negative ion colloid particulate attract each other and neutralize colloid surface charge. Because of the more coiled structure, chitosan polymer is able to compress pervation layer to take steady.In virtue of charge neutralization and adsorption and bridge connection effect so as to produce larger and denser flocs and affluent–NH_2 and–OH was used as absorbent for heavy metals.
Technologies for dye removal have been investigated, such as the electrolysis coagulation, chemical oxygenation, those processed condition is strict, the stability is bad. The article intends to introduce the authors’experimental study on four kinds of adsorbents which are made by chitosan-coated bentonite , chitosan-coated pearl, carboxymethyl chitosan-coated bentonite and carboxymethyl chitosan-coated pearl .The ability of chitosan-coated bentonite for the removal of reactive dye ,namely reactive red B-3G, blue B-2GLN, black B-GRFN, green B-4BLN,from aqueous solution has been studied. The experimental equilibrium data have been analyzed using the linearized forms of Langmuir, Freundlich isotherms .The Langmuir isotherm was found to provide the best theoretical correlation of the experimental data for the adsorption of all four reactive dyes. The monolayer adsorption capacities were determined to be11.850、7.760、7.276、8.362mg of dye per gram of chitosan-coated bentoniteadsorbent,respectively to four dyes. The results would provide a theoretical basisfor utilizing natural material to extract heavy metals from the contaminated soils.The adsorption of dyes onto Carboxymethyl chitosan adsorbent was expensiveprocess with high capacities. The paper also studied the application of adsorptionof Acid Brilliant Scarlet GR onto Chitosan-coated cellulose adsorbent has beenstudied. It was a fast process and K_1=0.884 h~(-1). in Lagergren equation.
The adsorption of BSA onto sphere Chitosan polymer has been experimented.Effect of amount of agents, pH value, adsorption time and ionic strength werestudied. The research results for coagulation of dairy producted wastewatersshow that the recovery efficiency of protein by chitosan was efficient. Theexperience of adsorption of Cd~(2+) and Al(Ⅲ)showed that the adsorption was a fastprocess with 254.5mg·g~(-1),49.0mg·g~(-1).capacity. Chitosan-Cd(Ⅱ), Chitosan- Al(Ⅲ)PPwas synthesized and FTIR, XPS analysis indicates that the adsorption was thecoordination of -NHB2 Band -OH groups of Chitosan to Cd~(2+).
The study assessed the feasibility of the application of chitosan for thecoagulation of kaolinite colloidal particles. The pH effect on the coagulationefficiency of chitosan is insignificant. The evidence infers that chargeneutralization is not a major mechanism controlling the formtion of floc forchitosan coagulation and the water conservancy condition is the key factorcongealed. Chitosan was used to enhance the flocculation treatment of thesurface water，which is the raw water of Yellow River in Zheng Zhou bypolymeric aluminum chloride (PAC).The improvement of removal efficiency ofturbidity and COD indicated that chitosan could enhance the flocculationtreatmen by PAC significantly. When PAC dosage is 35 mg·l~(-1), CTS dosage is0.15 mg·l~(-1), the effect of flocculation is better. Zeta potential instrument andScanning electron microscope were used to test Zeta potential and observe thestructure of flocs and infer flocculation mechanism was interpartical bridgingrather than the electrical neutralization by prositive charge. The floc wasobserved with microscope and image analysis system and the result show thatvariation in fractal dimension can make good response to flocculation level andPAC,PAC/CTS was 1.294,1.385 respectively.
The effect of the dosage of flocculants on activated sludge dewatering is analyzed through the determination of sludge specific resistance to filtration . Sludge dewatering behaviors conditioned on PAC, CTS and composite flocculants have been compared. The results show all the conditioning agent have help to sludge dewatering .Compared with Polymeric aluminum , Chitosan and PAC/CTS composite coagulant, the optimum coagulant with its optimum dosage is obtained . PAC/CTS can greatly reduce the sludge specific resistance and improves the sludge dewatering performance largely while the clarity of the filtrate was high. While designing the dewatering and drying process of sludge water from water works, we can ignore the coagulation process, and utilize fly ash of power plant as the conditioner of sludge from water works directly.
引文
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