表面活性剂对偶氮染料光催化氧化降解的影响研究
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摘要
H_2O_2/草酸铁光催化氧化体系是Fenton体系较为先进的高级氧化技术,偶氮染料和表面活性剂是印染废水中的重要组成部分,因此关于表面活性剂存在下偶氮染料在水中的脱色降解行为的研究对于印染废水的处理和利用更具有重要的现实意义。
本文分别选择三种偶氮类活性染料(C.I.活性红195、C.I.活性蓝222和C.I.活性黄145)和三种偶氮类酸性染料(C.I.酸性黑234、C.I.媒介黑9和C.I.酸性橙156)作为模拟污染物,利用H_2O_2/草酸铁光催化氧化体系研究了阴离子表面活性剂十二烷基苯磺酸钠(SDBS)和十二烷基硫酸钠(AS)以及非离子表面活性剂壬基酚聚氧乙烯醚(OP-10)和失水山梨醇脂肪酸酯聚氧乙烯醚(TW-80)对上述染料脱色降解反应的影响情况,重点考察了表面活性剂的浓度和种类对染料脱色率的影响。利用紫外可见光谱法研究了表面活性剂自身降解性能及其与偶氮染料在水溶液中的相互作用,同时采用最大气泡法测定了染料脱色反应过程中溶液表面张力的变化。最后通过紫外可见光谱法分析了表面活性剂存在条件下偶氮染料分子中芳香环结构在脱色降解过程中的变化。
结果表明,SDBS的加入对染料的脱色反应起到抑制作用,当SDBS的浓度处于5-7mmol/L范围内时,随着SDBS浓度的增加其对染料的抑制作用增强,浓度超过7mmol/L后SDBS浓度的变化对染料的影响作用不大。当OP-10的浓度为0.20mmol/L时,其对两种染料的脱色抑制作用最强,浓度超过0.20mmol/L后,OP-10对所选染料的抑制作用减缓或有所促进。表面活性剂对染料脱色降解反应的影响涉及到两个方面的因素,其一是表面活性剂的存在使得H_2O_2的分解率降低,其二是表面活性剂与染料竞争羟基自由基的作用。光辐射强度的大小并未明显改变SDBS和OP-10对染料的影响趋势,但是光辐射强度越大,染料的脱色率降解程度越大。Na_2SO_4的存在并未改变SDBS和OP-10对染料的脱色率反应的影响程度,NaCl和SDBS或OP-10的协同效应对染料脱色率的抑制作用增强。在表面活性剂存在条件下,染料的脱色反应仍符合假一级动力学反应的特征,SDBS的加入使得活性染料的动力学曲线分为两个部分。通过紫外可见光谱法发现表面活性剂的存在对偶氮染料分子中芳香环结构的抑制作用较偶氮键的抑制作用大,抑制作用随着表面活性剂浓度的提高而增强。
Treatment of dyeing water pollution is a major task of environmental protection. Among the treatment techniques,the method of H_2O_2/ferrioxalate photocatalytic oxidation system had drawn much attention.
Three reactive dyes with azo structure including C.I.Reactive Red195,C.I. reactive blue 222 and C.I.reactive yellow 145,and three kinds of acid dyes with azo structure,including C.I.acid black 234,C.I.mordant black 9 and C.I.acid orange 156 were chosen as the model pollutants for simulative contamination in this experiment. Four kinds of surfacants namely sodium dodecylbnzene sulfonate(SDBS),sodium lauryl sulfate(AS),Polyoxyethylene nonyl phenyl ether(OP-10)and Tween-80 (TW-80)were also used for simulative contamination,Some factors effecting the decoloration of azo dyes such as the type and concentrations of surfactants,various light intension were examined with respect to decoloration percentage.In order to have a better insight into the degradation of azo dyes in the presence of surfactants, the method of UV-visible-spectrum was introduced to discuss the degradation of surfactant and the interaction between surfactants and azo dyes in aqueous.
The results indicated that there is the significant interaction between nonioinc surfacant molecules(OP-10 and TW-80)and azo dyes,especially acid dyes.On the other hand,it is found that little interaction between anioinc surfacant molecules (SDBS and AS)and azo dyes.This is mainly becaues of the big difference in molecular structure of azo dyes.The decoloration could be limited(reduced,inhabited) in the presence of SDBS and in the concentration varying from 5-7.0mmol/L, meanwhile,the effect of limite increased with increasing the concentration of SDBS. The restraining for reactive dye 195 decoloration reached a peak when the concentration of OP-10 was 0.20mmol/L,over this concentration,the effect of restraining was reduced.The decoloration of black acid dye 234 was inhabited in the presence of OP-10 concentration under CMC,and accelerated over CMC.
The degradation of azo dyes are determined by two factors,One was that the rate of H_2O_2 decomposing was reduced in the presence of surfactant;another was that there was competition between SAA and dyes for hydroxyl radicals.When the concentration of SAA was below CMC concentration,surfactant can be easily degradated and contested for hydroxyl radicals with dyes strongly.When the concentration of SAA was more than CMC,the degradation of surfactant was carried out with difficulty.After experiment,it could be seen that the strength of light irradiation as well as Na_2SO_4 couldn't influence dyes degradation with SDBS and OP-10 respectively,but high light irradiation caused increased degradation of dyes.
本文分别选择三种偶氮类活性染料(C.I.活性红195、C.I.活性蓝222和C.I.活性黄145)和三种偶氮类酸性染料(C.I.酸性黑234、C.I.媒介黑9和C.I.酸性橙156)作为模拟污染物,利用H_2O_2/草酸铁光催化氧化体系研究了阴离子表面活性剂十二烷基苯磺酸钠(SDBS)和十二烷基硫酸钠(AS)以及非离子表面活性剂壬基酚聚氧乙烯醚(OP-10)和失水山梨醇脂肪酸酯聚氧乙烯醚(TW-80)对上述染料脱色降解反应的影响情况,重点考察了表面活性剂的浓度和种类对染料脱色率的影响。利用紫外可见光谱法研究了表面活性剂自身降解性能及其与偶氮染料在水溶液中的相互作用,同时采用最大气泡法测定了染料脱色反应过程中溶液表面张力的变化。最后通过紫外可见光谱法分析了表面活性剂存在条件下偶氮染料分子中芳香环结构在脱色降解过程中的变化。
结果表明,SDBS的加入对染料的脱色反应起到抑制作用,当SDBS的浓度处于5-7mmol/L范围内时,随着SDBS浓度的增加其对染料的抑制作用增强,浓度超过7mmol/L后SDBS浓度的变化对染料的影响作用不大。当OP-10的浓度为0.20mmol/L时,其对两种染料的脱色抑制作用最强,浓度超过0.20mmol/L后,OP-10对所选染料的抑制作用减缓或有所促进。表面活性剂对染料脱色降解反应的影响涉及到两个方面的因素,其一是表面活性剂的存在使得H_2O_2的分解率降低,其二是表面活性剂与染料竞争羟基自由基的作用。光辐射强度的大小并未明显改变SDBS和OP-10对染料的影响趋势,但是光辐射强度越大,染料的脱色率降解程度越大。Na_2SO_4的存在并未改变SDBS和OP-10对染料的脱色率反应的影响程度,NaCl和SDBS或OP-10的协同效应对染料脱色率的抑制作用增强。在表面活性剂存在条件下,染料的脱色反应仍符合假一级动力学反应的特征,SDBS的加入使得活性染料的动力学曲线分为两个部分。通过紫外可见光谱法发现表面活性剂的存在对偶氮染料分子中芳香环结构的抑制作用较偶氮键的抑制作用大,抑制作用随着表面活性剂浓度的提高而增强。
Treatment of dyeing water pollution is a major task of environmental protection. Among the treatment techniques,the method of H_2O_2/ferrioxalate photocatalytic oxidation system had drawn much attention.
Three reactive dyes with azo structure including C.I.Reactive Red195,C.I. reactive blue 222 and C.I.reactive yellow 145,and three kinds of acid dyes with azo structure,including C.I.acid black 234,C.I.mordant black 9 and C.I.acid orange 156 were chosen as the model pollutants for simulative contamination in this experiment. Four kinds of surfacants namely sodium dodecylbnzene sulfonate(SDBS),sodium lauryl sulfate(AS),Polyoxyethylene nonyl phenyl ether(OP-10)and Tween-80 (TW-80)were also used for simulative contamination,Some factors effecting the decoloration of azo dyes such as the type and concentrations of surfactants,various light intension were examined with respect to decoloration percentage.In order to have a better insight into the degradation of azo dyes in the presence of surfactants, the method of UV-visible-spectrum was introduced to discuss the degradation of surfactant and the interaction between surfactants and azo dyes in aqueous.
The results indicated that there is the significant interaction between nonioinc surfacant molecules(OP-10 and TW-80)and azo dyes,especially acid dyes.On the other hand,it is found that little interaction between anioinc surfacant molecules (SDBS and AS)and azo dyes.This is mainly becaues of the big difference in molecular structure of azo dyes.The decoloration could be limited(reduced,inhabited) in the presence of SDBS and in the concentration varying from 5-7.0mmol/L, meanwhile,the effect of limite increased with increasing the concentration of SDBS. The restraining for reactive dye 195 decoloration reached a peak when the concentration of OP-10 was 0.20mmol/L,over this concentration,the effect of restraining was reduced.The decoloration of black acid dye 234 was inhabited in the presence of OP-10 concentration under CMC,and accelerated over CMC.
The degradation of azo dyes are determined by two factors,One was that the rate of H_2O_2 decomposing was reduced in the presence of surfactant;another was that there was competition between SAA and dyes for hydroxyl radicals.When the concentration of SAA was below CMC concentration,surfactant can be easily degradated and contested for hydroxyl radicals with dyes strongly.When the concentration of SAA was more than CMC,the degradation of surfactant was carried out with difficulty.After experiment,it could be seen that the strength of light irradiation as well as Na_2SO_4 couldn't influence dyes degradation with SDBS and OP-10 respectively,but high light irradiation caused increased degradation of dyes.
引文
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