偶氮染料的太阳光催化氧化降解及其染色废水的回用
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摘要
印染废水的排放标准越来越严格,纺织工业面临的严峻形势是染料对水体的污染问题。光催化氧化技术作为一种高级氧化技术,近年来在染料废水处理中得到广泛的关注。本论文利用草酸盐络合物/过氧化氢体系,在太阳光辐射条件下对六种偶氮染料进行光催化氧化研究。首先考察了铁离子浓度、草酸浓度和过氧化氢浓度对染料脱色降解性能的影响。其次研究了无机盐、表面活性剂和太阳光强度等因素与染料光催化脱色降解以及动力学反应速率常数的之间的关系。比较了太阳光与人工光源对染料光催化作用的差异;并借助紫外—可见光谱(UV-VIS)和总有机碳(TOC)分析了染料脱色降解的反应过程。最后,使用中温型活性染料对棉织物染色加工,并利用上述技术对其染色废水进行脱色降解和回用研究。实验结果表明:铁离子浓度增加有利于染料光催化反应的进行;草酸和过氧化氢的用量的适当增加也有对染料的光催化反应有促进作用。无机盐对染料的光催化降解有抑制作用,并随着无机盐浓度的提高,其作用随之增加;相同的条件下,氯化钠的抑制作用最显著,硫酸钠次之,硝酸钠最小。表面活性剂在其临界胶束浓度以下,其对染料脱色降解的影响相对较小;但是当其浓度超过临界胶束浓度,明显地降低染料脱色率。一般而言,太阳光的强度越高,越有利于染料的脱色降解;在相同的反应条件下,在晴天时染料的脱色率明显高于阴天时染料的脱色率。在此催化氧化体系中,染料的脱色降解反应可以用假一级动力学反应模型来描述,并且无机盐的存在和太阳光强度的增加并没有影响这种反应模型。利用此技术可以实现活性染料废水的脱色降解,并将脱色后的废水(简称新水Ⅰ和新水Ⅱ)可以作为染色介质回用于棉织物的活性染料染色工艺中。其染色后织物与自来水为染色介质的染色织物的总色差(DE)小于1.5,符合商业化要求,此外染色织物牢度可以达到四级标准。
Since discharge limits are becoming stricter for industry wastewater textile manufactures are searching efficient and economical methods of pollution reduction. The technique of pHoto-catalytic oxidation is a new kind of water treatment process with great potential especially in the dyeing wastewaters degradation for its outstanding effect. This paper mainly investigated the pHoto-catalytic degradation of six azo dyes based on ferrioxalate oxalite/H_2O_2. Firstly, study on Fe3+, oxalic acid and H_2O_2 concentration are discussed in details. Secondly, the relation between inorganic salts, surfactants, solar irradiation and discoloration, reaction kinetics value was investigated. The different effect of solar and model solar in the ferrous oxalate complex/H_2O_2 on degradation azo dyes had been contrasted. In addition, the process of degradation was shown by UV-Vis spectrum and TOC. Finally, three reactive dyes containing two reactive groups in aqueous solutions were dyed fabric, the dyeing wastewaters carried out by this solar catalytic degradation technology and recycling of wastewater. The experimentation results indicated that the increase concentration of Fe3+ had accelerated the dyeing degradation, while the oxalic acid and H_2O_2 concentration had an optimization value. The more or less blocked the dye discoloration and degradation. Inorganic salts had restrained the degradation of dyes, the more of its concentration the worse the dyeing degradation. In the same condition, NaCl had the most restrained effect on dyeing degradation, next Na_2SO_4;the least was NaNO_3 Surfactants have a specific affected on dyeing discoloration, if its concentration less than C.M.C, it had a faint control, if its concentration more than C.M.C, it had a prominent control. Generally speaking, the higher the solar irradiance, the faster the discoloration of dyes in water. In the same condition, dyes were more efficiency degradated in sunny than in cloudy. It was found that the degradation of the dyes followed a pseudo-first order kinetic model at different solar irradiance and the inorganically salts in ferrioxalate oxalite/H_2O_2. Reactive dyes dyed fabric and produced wastewaters, which could be degradated by this pHoto catalytic technology, and the gained water (new water Ⅰ and Ⅱ) can be recycled in the reactive dyes dyeing process. The results DE* less than 1.5, contrasted fabric dyed by new water Ⅰ & Ⅱ with tap water, attained commerce requirement. In addition, new water Ⅰ & Ⅱ did not affect fabric other fasten and gained four grade standard according to corresponding nation standard.
Since discharge limits are becoming stricter for industry wastewater textile manufactures are searching efficient and economical methods of pollution reduction. The technique of pHoto-catalytic oxidation is a new kind of water treatment process with great potential especially in the dyeing wastewaters degradation for its outstanding effect. This paper mainly investigated the pHoto-catalytic degradation of six azo dyes based on ferrioxalate oxalite/H_2O_2. Firstly, study on Fe3+, oxalic acid and H_2O_2 concentration are discussed in details. Secondly, the relation between inorganic salts, surfactants, solar irradiation and discoloration, reaction kinetics value was investigated. The different effect of solar and model solar in the ferrous oxalate complex/H_2O_2 on degradation azo dyes had been contrasted. In addition, the process of degradation was shown by UV-Vis spectrum and TOC. Finally, three reactive dyes containing two reactive groups in aqueous solutions were dyed fabric, the dyeing wastewaters carried out by this solar catalytic degradation technology and recycling of wastewater. The experimentation results indicated that the increase concentration of Fe3+ had accelerated the dyeing degradation, while the oxalic acid and H_2O_2 concentration had an optimization value. The more or less blocked the dye discoloration and degradation. Inorganic salts had restrained the degradation of dyes, the more of its concentration the worse the dyeing degradation. In the same condition, NaCl had the most restrained effect on dyeing degradation, next Na_2SO_4;the least was NaNO_3 Surfactants have a specific affected on dyeing discoloration, if its concentration less than C.M.C, it had a faint control, if its concentration more than C.M.C, it had a prominent control. Generally speaking, the higher the solar irradiance, the faster the discoloration of dyes in water. In the same condition, dyes were more efficiency degradated in sunny than in cloudy. It was found that the degradation of the dyes followed a pseudo-first order kinetic model at different solar irradiance and the inorganically salts in ferrioxalate oxalite/H_2O_2. Reactive dyes dyed fabric and produced wastewaters, which could be degradated by this pHoto catalytic technology, and the gained water (new water Ⅰ and Ⅱ) can be recycled in the reactive dyes dyeing process. The results DE* less than 1.5, contrasted fabric dyed by new water Ⅰ & Ⅱ with tap water, attained commerce requirement. In addition, new water Ⅰ & Ⅱ did not affect fabric other fasten and gained four grade standard according to corresponding nation standard.
引文
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