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铁氮配合物的制备及其光催化降解腈纶废水的研究

Study on Preparation of New-type Photo-catalyst Iron Nitrogen Complex and Its Application in the Degradation of Acrylic Fiber Wastewater under Visible Light Irradiation

【作者】 李晓静

【导师】 赵朝成; 耿春香;

【作者基本信息】 中国石油大学 , 环境科学, 2008, 硕士

【摘要】 本文以寻找更适合光催化处理腈纶废水的方法和研制可以应用于腈纶废水处理的光催化剂为目标,进行了催化剂的制备及光催化的研究。实验制备了一种全新的、具有高光催化活性、高稳定性和免分离固相型Fenton光催化剂,该催化剂是将铁离子溶液负载到树脂上制成一种新型的固相催化剂。在制备研究中,以腈纶废水为研究对象,对各种负载型铁配合物进行了筛选,确定出其最佳合成条件:由0.4molFe2+配制成的溶液负载到30g聚苯乙烯/二乙烯苯的螯合型树脂上(D463)。通过对该催化剂处理腈纶废水的影响因素考察,得出处理腈纶废水时最佳条件为:H2O2浓度为55mmol·L-1,催化剂用量为10g·L-1,最佳pH值范围为3~5,COD降解率可达48.95%左右。此催化剂的研究使Fenton光催化处理污染物系统成为一种在固/液两相进行的无须预先调整待处理水的pH值,铁离子达到零排放的高效、简便的流动处理体系。实验研究了一种全新的、具有可见光光催化活性、高稳定性和免分离固相型光催化剂,该催化剂是将铁氮配合物溶液负载到树脂上制成一种新型的固相催化剂。以腈纶废水为研究对象,负载型铁氮配合物的制备,对各种负载型铁氮配合物进行了筛选,确定出一种固相催化剂及最佳合成条件:由1,10菲啰啉和Fe2+配制成的有机配合离子负载到聚甲基丙烯酸、聚甲基丙烯酸甲酯/二乙烯苯阳离子交换树脂上(D113),每克树脂可负载6×10-4mol的有机配合离子,菲啰啉/Fe2+摩尔比为2:1,有机配合离子pH值范围在3~3.5之间;用该负载型铁氮配合物处理腈纶废水的影响因素进行研究,得出处理腈纶废水时最佳条件为:H2O2浓度为44mmol·L-1,催化剂用量为5g·L-1,光照时间4h后腈纶废水COD降解率可达68.7%。实现了在温和的反应条件下,即常温、常压、宽pH范围进行反应,又能够被可见光激发,充分利用可见光。并且催化剂的化学性质稳定,可重复使用。实验得出了Fenton类光催化处理腈纶废水的最佳反应条件。通过比较,固相型催化剂在回收利用,COD降解率,可见光相应和生物可生化性方面都得到了改进。

【Abstract】 Aiming to search methods and develop a sort of catalyst of handling Acrylic Fibers wastewater more effectively, two sorts of solid-phase catalyst were prepared, the loading conditions of preparing catalyst and affecting factor of treating the wastewater were investigated in the process of photocatalytic degradation of Acrylic Fibers wastewater.A new solid-phase Fenton-type catalyst of high photocatalytic activity, high stability and dispense with separation were prepared, which is made from loading the iron solution onto the resin. The best loading conditions of preparing catalyst and affecting factor of treating wastewater were investigated in the process of photocatalytic degradation of Acrylic Fibers wastewater.The best conditions of preparing catalyst are as follows: loading ferrous solution onto the resin of polystyrene / divinylbenzene the chelating resin (D463). The best reaction condition of treating wastewater: the concentration of H2O2 is 55mmol·L-1, the amount of catalyst is 10g·L-1, the pH range is 3-5, the ratio of COD degradation is up to 48.95%.It becomes a efficient, simple mobile treatment system which dispense with pre-treating the wastewater pH and achieve zero emissions of ferrous ion by this catalyst in Fenton photocatalytic system.A new solid-phase type catalyst of high visible light photocatalytic activity, high stability and dispense with separation were prepared, which is made from loading the ferrous nitrogen complexe solution onto the resin. The best loading conditions of preparing catalyst and affecting factor of treating wastewater were investigated in the process of photocatalytic degradation of Acrylic Fibers wastewater.The best conditions of preparing catalyst are as follows: 1,10 phenanthroline and Fe2+ formate organic ion complex was exchanged into cationic exchange resin with Polyallylmethacrylate, PMMA/divinylbenzene. Per gram of resin can be loaded 6×10-4mol of organic complex. The best molar ratio of phenanthroline / Fe2+ is 2:1 in a range of pH (3~3.5) when referred to acrylic fiber wastewater treatment, the concentration of H2O2 is 44mmol·L-1, and the amount of catalyst is 5g·L-1. After four hours’irradiation the COD degradation of acrylic fiber wastewater rate up to 68.7%.From the experiment, the best reaction condition of treatment on the wastewater of Acrylic by Fenton and UV/Fenton was got. By comparison, solid-phase catalyst in treating the wastewater have been improving in the aspects of the recovery and utilization, COD degradation rate, responsibility of visible light and biodegradation rate.

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