金属螯合物催化臭氧氧化腈纶废水典型污染物实验研究

发布时间：2018-03-30 19:35

  本文选题：金属螯合物　切入点：臭氧　出处：《东北石油大学》2017年硕士论文

【摘要】：我国腈纶废水排放量逐年增大,而且国内几乎所有腈纶废水处理没有达标而排放到邻近水域,使高浓度有毒污染物残留在水体中,通过不断的迁移、累积对废水排放地区的环境造成了严重破坏。国内外对腈纶废水处理虽然有不少研究,但是仅仅局限于腈纶废水的处理上,而没有深入到对腈纶废水典型污染物的降解研究,从而没有达到针对性处理的目的。论文着眼于废水典型污染物的研究,选出腈纶废水中比较有代表性的污染物丁二腈作为研究对象,利用金属螯合物催化臭氧法对丁二腈进行氧化,旨在找到一种能高效地氧化丁二腈的高级氧化法,为金属螯合物催化臭氧法处理腈纶废水提供技术支持,对推动臭氧法处理工艺的发展具有积极意义。论文采用金属螯合物催化臭氧法氧化丁二腈,利用亚铁离子催化臭氧产生具有强氧化能力的氧化剂羟基自由基(·OH),对丁二腈进行无选择性地氧化,以期达到良好的降解效果。论文首先简述金属离子催化臭氧理论以及络合作用的理论,为后续实验研究创建了理论基础。通过对三种体系氧化丁二腈效能的比较,选择金属螯合物催化臭氧体系。随后选择金属螯合物。接着进行丁二腈氧化效能的单因素实验研究和正交实验研究。最后进行可生化性及动力学研究。研究结果表明,Fe(II)(焦磷酸钠)螯合物催化臭氧体系氧化丁二腈效能最好。五种单因素下该体系对丁二腈的氧化效能为:随着Fe(II)离子浓度、气相臭氧投加浓度和水力停留时间增加,氧化效能呈由快到慢的上升趋势;金属离子协同作用对氧化效能的影响较小;初始pH值的影响呈持续增大的趋势;丁二腈浓度的变化对金属螯合物催化效能的影响较小。正交实验分析可知,对于选定的四种影响因素主次顺序为水力停留时间(HRT)、Fe(II)离子浓度、初始pH值、气相臭氧投加浓度,HRT、Fe(II)离子浓度对实验结果有显著影响,实验最佳条件为初始pH值为7、Fe(II)离子浓度为0.2mmol/L、气相臭氧投加浓度为25~30mg/L、HRT为120min。在最佳条件下对丁二腈进行三次平行氧化实验,当HRT为120min时,丁二腈的平均去除率为72.4%。丁二腈溶液的可生化性能提高,B/C比值由0.18上升到0.46。此外,金属螯合物催化臭氧氧化丁二腈符合假一级动力学,初始pH值在1~7范围内,综合反应速率常数在0.00486~0.00869(min)-1之间。
[Abstract]:The discharge of acrylic fiber wastewater in China is increasing year by year, and almost all the domestic acrylic fiber wastewater treatment does not meet the standards and discharge to the adjacent waters, so that high concentration of toxic pollutants remain in the water, through continuous migration,The accumulation caused serious damage to the environment in the waste water discharge area.Although there is a lot of research on the treatment of acrylic fiber wastewater at home and abroad, it is limited to the treatment of acrylic fiber wastewater, but does not go deep into the study of degradation of typical pollutants in acrylic fiber wastewater, thus the purpose of targeted treatment has not been achieved.This paper focuses on the study of typical pollutants in wastewater and selects the representative pollutant succinonitrile in acrylic fiber wastewater as the research object and uses metal chelate to catalyze the oxidation of butadionitrile by ozone method.In order to find an advanced oxidation method which can oxidize succinonitrile efficiently and provide technical support for metal chelate catalytic ozone treatment of acrylic fiber wastewater, it is of positive significance to promote the development of ozone treatment process.In this paper, metal chelates were used to catalyze the oxidation of succinonitrile by ozone, and iron ion was used to catalyze ozone to produce oxidizing oxidant hydroxyl radical (OHN), which was used to oxidize succinonitrile nonselectively, in order to achieve a good degradation effect.Firstly, the theory of metal ion catalyzing ozone and the theory of complexation are briefly introduced, which provides a theoretical basis for further experimental study.The metal chelate catalytic ozone system was selected by comparing the performance of the three systems in the oxidation of succinonitrile.Then the metal chelate was selected.Then the single factor and orthogonal experiments were carried out on the oxidation efficiency of succinonitrile.Finally, the biodegradability and kinetics were studied.The results showed that the oxidation of succinonitrile was the best in the ozone system catalyzed by the chelate (sodium pyrophosphate).The oxidation efficiency of the system is as follows: with the concentration of Fe2 +, the concentration of gas phase ozone and HRT increase, and the oxidation efficiency increases from fast to slow.The effect of metal ion synergism on the oxidation efficiency was small; the effect of initial pH value was increasing; and the catalytic efficiency of metal chelate was less affected by the change of succinonitrile concentration.The orthogonal experiment results show that the primary and secondary order of the four factors are the HRT (HRT) FeII) ion concentration, the initial pH value and the gas phase ozone concentration (HRT) FeII) ion concentration, which have a significant effect on the experimental results.The optimum conditions are as follows: the initial pH value is 7% Fe2) ion concentration is 0.2 mmol / L, and the gas phase ozone concentration is 25 ~ 30 mg / L ~ (-1) HRT = 120 min.Under the optimum conditions, the average removal rate of succinonitrile was 72.4 when HRT was 120min.The biodegradability of succinonitrile solution increased from 0.18 to 0.46.In addition, the metal chelate catalyzed ozone oxidation of butylene nitrile accords with pseudo-first-order kinetics, the initial pH value is in the range of 1 ~ 7, and the comprehensive reaction rate constant is between 0.00486~0.00869(min)-1.
【学位授予单位】：东北石油大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：X783.4
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本文编号：1687338