催化臭氧化水中有机物机理研究
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摘要
本文首先综述了臭氧的物理化学性质和在水处理方面的应用,提出了本论文的研究目的.研究内容主要包括四部分:O_3/UV催化臭氧化降解水中有机物的机理研究;Fe~(2+)/Fe~(3+)均相催化臭氧化苯酚的研究;MnO_2催化臭氧化降解苯甲酸钠.
第三章中,实验研究了O_3/UV催化臭氧化降解水中有机物的机理.初步证实O_3/UV产生HO·的作用机理为:O_3+H2O→H_2O_2+O_2;H_2O_2→2·OH.UV能够促使溶解臭氧产生H_2O_2,进而生成羟基自由基,当对H_2O_2水溶液鼓O_2时,UV对H_2O_2的分解作用明显加快.在O_3/UV降解技术中,当目标有机物是对自由基链反应具有较好促进作用的乙醇酸时,即使是较弱的引发反应,也能使乙醇酸很好地降解;而当目标有机物是对自由基链反应具有抑制作用的乙酸时,引发足够量的羟基自由基(OH-,H_2O_2)是乙酸得到较好降解的必要条件.目标有机物(如芳族类和带不饱和键的化合物)在臭氧化过程中形成中间产物H_2O_2是O_3/UV降解效率提高的关键因素,其直接导致体系形成O_3/H_2O_2和H_2O_2/UV这2种高级氧化技术,从而提高体系产生羟基自由基的效率.
第四章的研究结果表明,在一定条件下,在苯酚的臭氧化降解过程中,臭氧分子与苯酚及苯氧负离子的直接反应是苯酚降解的主要原因.Fe~(2+)和Fe~(3+)对臭氧化降解苯酚均具有催化作用,其中Fe~(2+)的催化效果更佳.Fe~(2+)催化降解苯酚的机理是:苯酚在臭氧化降解过程中产生了H_2O_2,分别同臭氧和Fe~(2+)形成了O_3/H_2O_2和Fenton体系,促进了苯酚的去除.不同体系R_(ct)的大小:O_3/Fe~(2+)＞O_3/Fe~(3+)＞_O3.这个结果也与苯酚的降解效果相一致.
第五章的研究结果表明,单独使用臭氧降解苯甲酸钠时,虽然在一定条件下苯甲酸钠可以被完全降解,但体系COD仍有较高的残留.加入MnO_2对COD的去除有明显的提高(由原来的79%提高到94%),显示了较好的催化性能.O_3/MnO_2体系的R_(ct)大于单独臭氧化.MnO_2催化臭氧化降解苯甲酸钠的机理是:MnO_2和草酸形成了草酸锰复合物,提高了臭氧对小分子有机酸的反应活性,致使反应溶液pH升高,进而加速臭氧分解.通过加入自由基猝灭剂,发现·OH也是提高体系矿化率的重要原因.
The physical chemistry properties of ozone and its application in water treatment were reviewed,the research objection was proposed too. There were three parts in this paper:Mechanism of UV catalytic ozonation of organic compound in solution;Fe~(2+)/Fe~(3+)homogeneous catalytic ozonation of phenol;MnO_2 catalytic ozonation of Sodium Benzoate. In chapterⅢ,the mechanism of producing of OH in O3/UV was proposed as follows:O_3 + H_2O→H_2O_2 + O_2;H_2O_2→2·OH.UV can promote the dissolved ozone to firstly produce H_2O_2,then the intermdiate H_2O_2 can react with dissolved ozone or decompose by UV to produce HO·.The experimental results also indicated that decomposition of H_2O_2 radiated by UV could be accerlated in the present of O_2.Furthermore,the characteristic of organic,which acts as promoter or inhibitor in the process of ozonation, also affects the degradation efficiency of O_3/UV directly,when glycolic acid,a promoter in ozonation,was degraded,the combination UV radiation with ozonation could remove it efficiency despite of less initiation reaction; however,when acetic acid,an inhibitor in ozonation,was degraded by O_3/UV,the removal rate of acetic acid was very low unless enough initiation of hydroxyl radical(OH~-,H_2O_2).The intermediate H_2O_2,has been proved to plays an important role in enhancement of degradation efficiency of O_3/UV.It resulted directly in the formation of two AOPs:O_3/H_2O_2和H_2O_2/UV systems,which both produce·OH efficiently.
The results in chapterⅣshow that the direct reactions between phenol(or C_6H_5O~-)and ozone are the main causes for degradation of phenol.Both Fe~(2+)and Fe~(3+)could improve the degradation efficiency of ozonation of phenol,and Fe~(2+)had higher activity in ozonation of phenol than Fe~(3+)had.The possible mechanism of Fe~(2+)homogeneous catalytic ozonation of phenol includes two reasons:O_3/H_2O_2 and Fenton system.In this system,the intermdiate H_2O_2 resulted in promoting the removal of phenol.The R_(ct)of different systems is:O_3/Fe~(2+)＞O_3/Fe~(3+)＞O_3,which is in accordance with their degradaton efficiencies of phenol.
The results in chapterⅤshow that the COD removal was not high in spite of the complete disappearance of Sodium Benzoate in specific time,indicating some compounds inert to ozone accumulated in solution. Addition of MnO_2 increased the degradation efficiency of COD by ozone obviously(from 79%to 94%).R_(ct)of different systems were calculated: O_3/MnO_2＞O_3.The mechanism of MnO_2 catalytic ozonation of Sodium Benzoate included two causes:(1)MnO_2 increased the reactive activity of organic acid with ozone;(2)adding MnO_2 cound increase the pH of solution,then high pH promoted the decomposition of ozone to produce·OH.The radical scavenger test confirmed the second cause.
第三章中,实验研究了O_3/UV催化臭氧化降解水中有机物的机理.初步证实O_3/UV产生HO·的作用机理为:O_3+H2O→H_2O_2+O_2;H_2O_2→2·OH.UV能够促使溶解臭氧产生H_2O_2,进而生成羟基自由基,当对H_2O_2水溶液鼓O_2时,UV对H_2O_2的分解作用明显加快.在O_3/UV降解技术中,当目标有机物是对自由基链反应具有较好促进作用的乙醇酸时,即使是较弱的引发反应,也能使乙醇酸很好地降解;而当目标有机物是对自由基链反应具有抑制作用的乙酸时,引发足够量的羟基自由基(OH-,H_2O_2)是乙酸得到较好降解的必要条件.目标有机物(如芳族类和带不饱和键的化合物)在臭氧化过程中形成中间产物H_2O_2是O_3/UV降解效率提高的关键因素,其直接导致体系形成O_3/H_2O_2和H_2O_2/UV这2种高级氧化技术,从而提高体系产生羟基自由基的效率.
第四章的研究结果表明,在一定条件下,在苯酚的臭氧化降解过程中,臭氧分子与苯酚及苯氧负离子的直接反应是苯酚降解的主要原因.Fe~(2+)和Fe~(3+)对臭氧化降解苯酚均具有催化作用,其中Fe~(2+)的催化效果更佳.Fe~(2+)催化降解苯酚的机理是:苯酚在臭氧化降解过程中产生了H_2O_2,分别同臭氧和Fe~(2+)形成了O_3/H_2O_2和Fenton体系,促进了苯酚的去除.不同体系R_(ct)的大小:O_3/Fe~(2+)＞O_3/Fe~(3+)＞_O3.这个结果也与苯酚的降解效果相一致.
第五章的研究结果表明,单独使用臭氧降解苯甲酸钠时,虽然在一定条件下苯甲酸钠可以被完全降解,但体系COD仍有较高的残留.加入MnO_2对COD的去除有明显的提高(由原来的79%提高到94%),显示了较好的催化性能.O_3/MnO_2体系的R_(ct)大于单独臭氧化.MnO_2催化臭氧化降解苯甲酸钠的机理是:MnO_2和草酸形成了草酸锰复合物,提高了臭氧对小分子有机酸的反应活性,致使反应溶液pH升高,进而加速臭氧分解.通过加入自由基猝灭剂,发现·OH也是提高体系矿化率的重要原因.
The physical chemistry properties of ozone and its application in water treatment were reviewed,the research objection was proposed too. There were three parts in this paper:Mechanism of UV catalytic ozonation of organic compound in solution;Fe~(2+)/Fe~(3+)homogeneous catalytic ozonation of phenol;MnO_2 catalytic ozonation of Sodium Benzoate. In chapterⅢ,the mechanism of producing of OH in O3/UV was proposed as follows:O_3 + H_2O→H_2O_2 + O_2;H_2O_2→2·OH.UV can promote the dissolved ozone to firstly produce H_2O_2,then the intermdiate H_2O_2 can react with dissolved ozone or decompose by UV to produce HO·.The experimental results also indicated that decomposition of H_2O_2 radiated by UV could be accerlated in the present of O_2.Furthermore,the characteristic of organic,which acts as promoter or inhibitor in the process of ozonation, also affects the degradation efficiency of O_3/UV directly,when glycolic acid,a promoter in ozonation,was degraded,the combination UV radiation with ozonation could remove it efficiency despite of less initiation reaction; however,when acetic acid,an inhibitor in ozonation,was degraded by O_3/UV,the removal rate of acetic acid was very low unless enough initiation of hydroxyl radical(OH~-,H_2O_2).The intermediate H_2O_2,has been proved to plays an important role in enhancement of degradation efficiency of O_3/UV.It resulted directly in the formation of two AOPs:O_3/H_2O_2和H_2O_2/UV systems,which both produce·OH efficiently.
The results in chapterⅣshow that the direct reactions between phenol(or C_6H_5O~-)and ozone are the main causes for degradation of phenol.Both Fe~(2+)and Fe~(3+)could improve the degradation efficiency of ozonation of phenol,and Fe~(2+)had higher activity in ozonation of phenol than Fe~(3+)had.The possible mechanism of Fe~(2+)homogeneous catalytic ozonation of phenol includes two reasons:O_3/H_2O_2 and Fenton system.In this system,the intermdiate H_2O_2 resulted in promoting the removal of phenol.The R_(ct)of different systems is:O_3/Fe~(2+)＞O_3/Fe~(3+)＞O_3,which is in accordance with their degradaton efficiencies of phenol.
The results in chapterⅤshow that the COD removal was not high in spite of the complete disappearance of Sodium Benzoate in specific time,indicating some compounds inert to ozone accumulated in solution. Addition of MnO_2 increased the degradation efficiency of COD by ozone obviously(from 79%to 94%).R_(ct)of different systems were calculated: O_3/MnO_2＞O_3.The mechanism of MnO_2 catalytic ozonation of Sodium Benzoate included two causes:(1)MnO_2 increased the reactive activity of organic acid with ozone;(2)adding MnO_2 cound increase the pH of solution,then high pH promoted the decomposition of ozone to produce·OH.The radical scavenger test confirmed the second cause.
引文
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