本文選題：二氯苯酚　切入點：十溴聯(lián)苯醚　出處：《哈爾濱工業(yè)大學(xué)》2015年碩士論文

【摘要】：鹵代有機物化學(xué)性質(zhì)穩(wěn)定,容易在生物體內(nèi)蓄積,并且具有較強的毒性和較高的三致效應(yīng)(致癌、致突變和致畸),其中有很大一部分被列為環(huán)境優(yōu)先控制的污染物。本研究以二氯苯酚(DCP)和十溴聯(lián)苯醚(BDE-209)作為代表,對其進行紫外輔助化學(xué)法的降解研究。DCP是我國自然水體中主要的污染物之一,BDE-209是應(yīng)用廣泛的阻燃劑,二者都可以對環(huán)境和人類健康造成嚴重危害。本實驗使用的紫外輔助化學(xué)法分為紫外催化濕式氧化法和紫外高級還原法兩種。通過單因素實驗優(yōu)化最佳降解條件,并在最優(yōu)條件下,進行脫鹵離子和中間產(chǎn)物的檢測,推測其降解機理。采用紫外催化濕式氧化法對DCP進行降解。研究表明,此方法對DCP降解效果顯著,對于濃度為50 mg/L的DCP溶液,在pH值為3,H_2O_2投加濃度為50μmol/L,CuSO_4的投加濃度為1 g/L,紫外光強度為3.5 W/m2的條件下,反應(yīng)40 min后,對DCP的去除率可達88.74%,在此條件下進行TOC和氯離子的測定,發(fā)現(xiàn)TOC去除率為69.9%,脫氯率為81.84%。說明此方法不僅有脫氯作用,還可將DCP開環(huán)礦化為CO2和H2O等。使用紫外高級還原法對DCP進行降解研究,選取Na_2SO_3和NaBH_4作為還原劑,發(fā)現(xiàn)NaBH_4的作用略強于Na_2SO_3,對于濃度為50 mg/L的DCP溶液,在pH值為12,NaBH_4的投加量為2 mmol/L,紫外光強度為3.5 W/m2的條件下,反應(yīng)60 min后DCP去除率為83.79%。對其TOC和氯離子進行測定,發(fā)現(xiàn)此方法對DCP的降解主要以脫氯為主,脫氯率為50.32%,TOC去除率僅為8.6%。在證明了紫外高級還原法顯著的作用后,選取更難降解的BDE-209作為目標(biāo)物,同樣選取Na_2SO_3和NaBH_4作為還原劑,發(fā)現(xiàn)NaBH_4的作用略強于Na_2SO_3,對于濃度為40 mg/L的BDE-209溶液,在pH值為12,NaBH_4的投加量為2 mmol/L,紫外光強度為3.5 W/m2的條件下,反應(yīng)60 min后BDE-209去除率為89.25%。使用GC-MS對中間產(chǎn)物進行檢測,發(fā)現(xiàn)其降解以脫溴為主,其中九溴、八溴聯(lián)苯醚是主要的中間產(chǎn)物,本反應(yīng)降解BDE-209主要以脫溴為主,而且會逐個脫掉溴原子。
[Abstract]:Halogenated organic compounds have stable chemical properties, easy to accumulate in organisms, and have strong toxicity and high triple-effect (carcinogenesis, carcinogenesis). Mutagenicity and teratogenicity, a large proportion of which are listed as environmentally priority control pollutants. In this study, dichlorophenol (DCP) and decabromodiphenyl ether (BDE-209) were used as examples. Degradation of BDE-209 by UV assisted chemical method. DCP is one of the main pollutants in natural water in China. BDE-209 is a widely used flame retardant. Both of them can cause serious harm to the environment and human health. The ultraviolet auxiliary chemical method used in this experiment is divided into two kinds: ultraviolet catalytic wet air oxidation method and ultraviolet advanced reduction method. The optimum degradation conditions are optimized by single factor experiment. Under the optimum conditions, the dehalogenation ions and intermediate products were detected, and the degradation mechanism was speculated. UV catalytic wet air oxidation method was used to degrade DCP. The results showed that the degradation effect of this method on DCP was remarkable. For DCP solution with 50 mg/L concentration, under the conditions of 50 渭 mol / L CUSO _ 4 and 50 渭 mol / L CUSO _ 4, the removal rate of DCP can reach 88.74% after 40 min reaction. Under these conditions, TOC and chloride ions are determined. The results show that the removal rate of TOC and dechlorination are 69.9 and 81.84 respectively. It shows that this method can not only dechlorinate, but also mineralize DCP into CO2 and H2O. The degradation of DCP is studied by ultraviolet advanced reduction method, and Na_2SO_3 and NaBH_4 are selected as reductants. It was found that the effect of NaBH_4 was slightly stronger than that of NaBH_4. For 50 mg/L DCP solution, the removal rate of DCP after 60 min reaction was 83.79 when the dosage of DCP was 2 mmol / L at pH 12 mg/L NaBHH4, and the UV intensity was 3.5 W/m2. It was found that the degradation of DCP by this method was mainly dechlorination, and the dechlorination efficiency was only 8.6. after proving the remarkable effect of ultraviolet advanced reduction method, the more difficult BDE-209 was chosen as the target, and the Na_2SO_3 and NaBH_4 were also selected as reducing agents. It was found that the effect of NaBH_4 was slightly stronger than that of NaBH_4. For 40 mg/L BDE-209 solution, the removal rate of BDE-209 was 89.25 when the dosage of BDE-209 was 2 mmol / L at pH 12 mg/L and UV intensity was 3.5 W/m2. GC-MS was used to detect the intermediate product. It was found that the degradation of BDE-209 was mainly debromination, in which pentabromyl and octabromodiphenyl ether were the main intermediate products. In this reaction, debrominated BDE-209 was mainly debrominated, and the bromine atoms were removed one by one.
【學(xué)位授予單位】：哈爾濱工業(yè)大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2015
【分類號】：X505

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