邻苯二甲酸酯DCHP和BBP的生物降解试验研究
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摘要
在综述国内外相关文献和大量试验的基础上,研究了曝气生物滤池(BAF)对环境激素类污染物邻苯二甲酸二环己酯(DCHP)和邻苯二甲酸丁基苄酯(BBP)的去除特性,初步探讨了其去除机理和生物降解途径。结果表明,生物滤柱可有效地去除水中微量的邻苯二甲酸二环己酯(DCHP)和邻苯二甲酸丁基苄酯(BBP),当水温为25℃,空床接触时间为8h时,生物滤柱对DCHP的去除率可达到96.3%,对BBP的去除率可达到95.7%;当水温为7℃,空床接触时间为8h时,生物滤柱对DCHP的去除率可达到79.3%,对BBP的去除率可达到83.5%;在人工配置的进水DCHP和BBP浓度为2mg/L左右时,经生物滤柱处理之后DCHP的出水浓度最低可降至0.05mg/L,BBP的出水浓度最低可降至0.09mg/L;生物滤柱对DCHP和BBP的去除率受水温、pH值和空床接触时间等多种因素的影响;温度越高,DCHP和BBP的去除率越大;由于微生物在代谢DCHP和BBP的过程中会产生邻苯二甲酸等酸性物质,出水pH值降低,去除率越大,进、出水pH值差值越大;随着空床接触时间(EBCT)的延长,反应器中DCHP和BBP的浓度逐渐降低,EBCT的增加延长了生物膜与有机物的接触时间,使微生物有更充足的时间利用水中的有机污染物;生物滤柱内微生物的生长繁殖受到水中有机物所能提供的能源和碳源等的影响,生物滤柱采用由下而上的进水方式,随着滤层高度的增加,水中的有机物逐渐减少,微生物数量因此减少,生物滤柱对DCHP和BBP的去除率的增加率逐渐减小;滤柱内陶粒填料上的生物膜在滤料表面以菌胶团形式存在,球状菌和短杆菌为主。GC/MS分析发现,DCHP的降解产物中含有邻苯二甲酸二己酯、邻苯二甲酸二丁酯、邻苯二甲酸单丁酯、邻苯二甲酸二甲酯和邻苯二甲酸等;BBP的降解产物中含有邻苯二甲酸二丁酯、邻苯二甲酸二甲酯和邻苯二甲酸等;据此推测DCHP的生物降解途径为:DCHP降解到邻苯二甲酸二丁酯后分两种途径进行,一种为邻苯二甲酸二丁酯分解为邻苯二甲酸单丁酯,再分解为邻苯二甲酸,另一种为邻苯二甲酸二丁酯分解为邻苯二甲酸二甲酯,再分解为邻苯二甲酸单甲酯,然后进一步生成邻苯二甲酸;最后生成二氧化碳和水;BBP的生物降解途径可能为:BBP分子支链上的苯环开裂生成邻苯二甲酸二丁酯,然后生成邻苯二甲酸二甲酯,进一步生成邻苯二甲酸,最后生成二氧化碳和水。
On the basis of summarizing the related references home and abroad,a great deal of experiments had been done to study removal characteristics of BAF on the Endocrine Disruptors Dicyclohexyl phthalate ester and butyl benzyl phthalate . Results show that the Biological filter column can effectively remove the water column trace DCHP and BBP, wiht a water temperature of 25℃and a empty bed contact time of 8h , the removal rate of DCHP could reach 96.3% ,and the BBP is 95.7% by the Biological filter column; with a temperature of 7℃and a empty bed contact time of 8h, then the removal rate of DCHP could reach up to 79.3%, and the BBP is 83.5%; When the DCHP and BBP’s concentration in manual configuration of water is about 2mg/L, after the Biological filter column,the outlet concentration of DCHP can decline to 0.05mg/L at the lowest,the BBP is 0.09mg/L;The removal rates of the Biological filter column to DCHP and BBP subject to water temperature, pH and empty bed contact time and other factors; The higher the temperature,the greater of the removal rate;because the process of microbial metabolize DCHP and BBP can produce phthalic acid and other acidic substances, The outlet water pH became lower, the greater of the removal rate,the bigger of the difference between the water inlet and outlet; as the extension of the empty bed contact time (EBCT), the concentrations of DCHP and BBP decreased gradually. the increase of EBCT extended the contact time of biofilm with organic matter. so that microbes have more time to use the organic pollutants in water; The growth and breeding of microbes in the biological filter column were affected by the energy and carbon source provided by the organic compounds in water. In upflow reactor, with the height of filtering layer increasing, the energy material cut down gradually,so the number of microbes also cut down with it,and the increase of removal of DCHP and BBP in the biological filter column decreased too. The biofilm of potsherd filling in the biological filter column exists in the form bacteria micelle, and mainly spherical bacteria and Brevibacterium are in that;By GC/MS analysis,it shows that,the degradation products of DCHP( Dicyclohexyl phthalate)containing Di-hexyl phthalate,Dibutyl phthalate, Monobutyl phthalate,Dimethyl phthalate, and Pathalic acid, etc.the degradation products of BBP(Butyl benzyl phthalate) containing Dibutyl phthalate,Dimethyl phthalate and Pathalic acid, etc. it can be inferred that the pathway of DCHP biological degradation was:after DCHP degradate to Dibutyl phthalate two ways maybe exist,one is that Dibutyl phthalate degradate to Monobutyl phthalate then Pathalic acid;the other way is that Dibutyl phthalate degradate to Dimethyl phthalate then Monomethyl phthalate, then Pathalic acid, and finally to Carbon dioxide and water; the pathways of BBP biological degradation could be that Benzene of the BBP branched-chain crack to Dibutyl phthalate, and then generate Dimethyl phthalate, then Pathalic acid, and finally to Carbon dioxide and water。
On the basis of summarizing the related references home and abroad,a great deal of experiments had been done to study removal characteristics of BAF on the Endocrine Disruptors Dicyclohexyl phthalate ester and butyl benzyl phthalate . Results show that the Biological filter column can effectively remove the water column trace DCHP and BBP, wiht a water temperature of 25℃and a empty bed contact time of 8h , the removal rate of DCHP could reach 96.3% ,and the BBP is 95.7% by the Biological filter column; with a temperature of 7℃and a empty bed contact time of 8h, then the removal rate of DCHP could reach up to 79.3%, and the BBP is 83.5%; When the DCHP and BBP’s concentration in manual configuration of water is about 2mg/L, after the Biological filter column,the outlet concentration of DCHP can decline to 0.05mg/L at the lowest,the BBP is 0.09mg/L;The removal rates of the Biological filter column to DCHP and BBP subject to water temperature, pH and empty bed contact time and other factors; The higher the temperature,the greater of the removal rate;because the process of microbial metabolize DCHP and BBP can produce phthalic acid and other acidic substances, The outlet water pH became lower, the greater of the removal rate,the bigger of the difference between the water inlet and outlet; as the extension of the empty bed contact time (EBCT), the concentrations of DCHP and BBP decreased gradually. the increase of EBCT extended the contact time of biofilm with organic matter. so that microbes have more time to use the organic pollutants in water; The growth and breeding of microbes in the biological filter column were affected by the energy and carbon source provided by the organic compounds in water. In upflow reactor, with the height of filtering layer increasing, the energy material cut down gradually,so the number of microbes also cut down with it,and the increase of removal of DCHP and BBP in the biological filter column decreased too. The biofilm of potsherd filling in the biological filter column exists in the form bacteria micelle, and mainly spherical bacteria and Brevibacterium are in that;By GC/MS analysis,it shows that,the degradation products of DCHP( Dicyclohexyl phthalate)containing Di-hexyl phthalate,Dibutyl phthalate, Monobutyl phthalate,Dimethyl phthalate, and Pathalic acid, etc.the degradation products of BBP(Butyl benzyl phthalate) containing Dibutyl phthalate,Dimethyl phthalate and Pathalic acid, etc. it can be inferred that the pathway of DCHP biological degradation was:after DCHP degradate to Dibutyl phthalate two ways maybe exist,one is that Dibutyl phthalate degradate to Monobutyl phthalate then Pathalic acid;the other way is that Dibutyl phthalate degradate to Dimethyl phthalate then Monomethyl phthalate, then Pathalic acid, and finally to Carbon dioxide and water; the pathways of BBP biological degradation could be that Benzene of the BBP branched-chain crack to Dibutyl phthalate, and then generate Dimethyl phthalate, then Pathalic acid, and finally to Carbon dioxide and water。
引文
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[12]陈丽旋,曾峰,罗丹玲等.城市道路灰尘中邻苯二甲酸酯污染特征研究.环境科学学报,2005,25(3):409-413
[13]莫测辉,蔡全英等.我国城市污泥中邻苯二甲酸醋的研究.中国环境科学,2001,21(4):362-366
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