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多溴联苯醚类物质辐射降解机理及其动力学研究
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摘要
本文首先综述了水中持久性有机污染物——多溴联苯醚(PBDEs)的特征、来源、国内外研究进展、治理概况和电子束、紫外降解持久性有机污染物在水污染治理中的研究进展,提出了本文的研究目的和意义。论文内容主要包括两个部分:利用紫外光或者电子束降解4-溴联苯醚的机理、动力学及其影响因素;紫外光解或者电子束辐解十溴联苯醚的降解机理、动力学及其影响因素,通过对4-溴联苯醚和十溴联苯醚这两类溴代苯醚有机物的紫外光解和电子束降解特性的分析,推测得知多溴联苯醚的紫外光解和电子束降解特性及途径。
     (1)无氧条件下,4-溴联苯醚在紫外光照下产生阳离子自由基,其阳离子自由基的生成速率k=2.67×10~6 s~(-1)·mol~(-1)·dm~3。当4-溴联苯醚溶液的pH>10.02,4-溴联苯醚在紫外光照下产生的阳离子自由基脱质子变为中性自由基。一定紫外光强范围内,4-溴联苯醚光解产物为苯醚和联苯酚两类有机物。初步推测无氧条件下,中性4-溴联苯醚溶液中,4-溴联苯醚紫外光解脱溴产生阳离子自由基,进一步反应生成苯醚和联苯酚等较稳定的中间体。4-溴联苯醚的溶液体系、初始pH值、初始浓度和光照时间对4-溴联苯醚降解的影响。
     利用电子束降解4-溴联苯醚。研究结果表明,电子束对4-溴联苯醚脱溴,进而降解具有明显的作用。实验进一步讨论了,4-溴联苯醚的溶液体系、初始pH值、初始浓度和辐照剂量对4-溴联苯醚降解的影响。
     (2)采用紫外光解十溴联苯醚。研究结果表明,十溴联苯醚与4-溴联苯醚光解特性相似,十溴联苯醚在紫外光照下脱溴,进而降解。实验进一步讨论了,十溴联苯醚光解的中间产物和光解机理,结合4-溴联苯醚的降解机理,推测多溴联苯醚的光解机理和特性。十溴联苯醚的溶液体系、初始pH值和光照时间对十溴联苯醚降解的影响。降解后的十溴联苯醚,溴离子被脱除,成为低溴代联苯醚。
     利用电子束降解十溴联苯醚。研究结果表明,电子束对十溴联苯醚脱溴,进而降解具有明显的作用。实验进一步讨论了,十溴联苯醚的溶液体系、初始pH值、辐解剂量对十溴联苯醚降解的影响。
     (3)采用多种分析手段(UV-VIS,pH,GC,HPLC,GC-MS)确定紫外光催化氧化或者电子束降解两类多溴联苯醚的中间产物。在4-溴联苯醚的降解过程中,主要分析了3种中间产物:联苯醚、对羟基联苯和邻羟基联苯。并推测了4-溴联苯醚主要的降解途径。
     在十溴联苯醚的降解过程中,主要分析了2种中间产物:联苯醚、八溴联苯醚。并推测了十溴联苯醚主要的降解途径。
A review of degradation of non-biodegradable persistent organic compounds and technique of photocatalysis or electron beam was firstly presented. And then the research aim was proposed. There are two parts in this paper: BDE-3 degradation by photocatalysis of UV irradiation or electron beam processes, proposed pathway of BDE-3 degradation by the process; BDE-209 degradation by photocatalysis of UV irradiation or electron beam processes, proposed pathway of BDE-209 degradation by the process.
     (1) The experiment of BDE-3 degradation, by photocatalsis of UV irradiation, shows that the synergistic effect exists on the decomposition of BDE-3 by EB. The effects of operating parameters, i.e. initial pH value, concentration of BDE-3, energy of UV, were also investigated. It is found that the structure of BDE-3 is destroyed and its biodegradability is improved.
     (2) The experiment of BDE-209 degradation, by photocatalsis of UV irradiation, shows that the synergistic effect exists on the decomposition of BDE-209 by EB. The effects of operating parameters, i.e. initial pH value, concentration of BDE-209, energy of UV, were also investigated. It is found that the structure of BDE-209 is destroyed and its biodegradability is improved.
     (3) Intermediates of BDE-3 and BDE-209 degradation by photocatalysis of UV irradiation were analyzed by some analytic technologies (UV-vis, pH value, GC, LC, GC-MS). Three products were identified: diphenylether, o-hydroxyphenyl, p-hydroxyphenyl. The pathway of BDE-3 degradation was discussed.
引文
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